Synthetic materials decorated with hydrogel coatings can accommodate the requirements of biological tissues for biocompatibility, lubricity, and flexibility. Nevertheless, these features may be subject to deterioration under long-term severe friction conditions. Inspired by Ambystoma mexicanum, a regenerative hydrogel coating to circumventing existing notions of wear resistance is presented, which can maintain a long-term lubricated and soft surface through the utilization of increment substances under abiotic mechanisms. The term regenerative refers to a process of directional differentiation without the use of external raw materials, whereby a hydrophobic plastic (PDHEA) is transformed into a hydrophilic hydrogel (PHEA) coating in response to external stimulation. Such a regenerative hydrogel coating can not only be repaired after local wear and reborn after full wear, but also be adjusted with the thickness and mechanical properties according to specific engineering requirements during differentiation. Furthermore, the regenerative hydrogel coating is applied for the surgery of artificial cartilage, with potential clinical applications such as long-acting protection of bone tissue.
| [1] |
Z. Liu, W. Li, L. Geng, et al., “Cross-Species Metabolomic Analysis Identifies Uridine as a Potent Regeneration Promoting Factor,” Cell Discovery 8, no. 1 (2022): 6.
|
| [2] |
H. B. D. Tran, C. Vazquez-Martel, S. O. Catt, et al., “4D Printing of Adaptable “Living” Materials Based on Alkoxyamine Chemistry,” Advanced Functional Materials 34, no. 23 (2024): 2315238.
|
| [3] |
T. Rajasooriya, H. Ogasawara, Y. Dong, J. N. Mancuso, and K. Salaita, “Force-Triggered Self-Destructive Hydrogels,” Advanced Materials 35, no. 52 (2023): 2305544.
|
| [4] |
X. Xu, Z. Fang, B. Jin, et al., “Regenerative Living 4D Printing via Reversible Growth of Polymer Networks,” Advanced Materials 35, no. 16 (2023): 2209824.
|
| [5] |
H. Zhang and Y. A. Hu, “A Statistical-Chain-Based Theory for Dynamic Living Polymeric Gels With Concurrent Diffusion, Chain Remodeling Reactions and Deformation,” Journal of the Mechanics and Physics of Solids 172 (2023): 105155.
|
| [6] |
Z. Wang, D. Ma, J. Liu, et al., “4D Printing Polymeric Biomaterials for Adaptive Tissue Regeneration,” Bioactive Materials 48 (2025): 370.
|
| [7] |
W. Liao, Y. Shi, Z. Li, and X. Yin, “Advances in 3D Printing Combined With Tissue Engineering for Nerve Regeneration and Repair,” Journal of Nanobiotechnology 23 (2025): 5.
|
| [8] |
Y. Pang, H. Wang, Y. Yao, et al., “An Injectable Self-Crosslinked Wholly Supramolecular Polyzwitterionic Hydrogel for Regulating Microenvironment to Boost Infected Diabetic Wound Healing,” Advanced Functional Materials 33, no. 36 (2023): 2303095.
|
| [9] |
R. Yang, B. Wang, X. Zhang, et al., “A Nucleobase-Driven Self-Gelled Hyaluronic Acid-Based Injectable Adhesive Hydrogel Enhances Intervertebral Disc Repair,” Advanced Functional Materials 34, no. 36 (2024): 2401232.
|
| [10] |
J. Wu, Z. Cui, Y. Su, et al., “Tuning on Passive Interfacial Cooling of Covalent Organic Framework Hydrogel for Enhancing Freshwater and Electricity Generation,” SusMat 4, no. 5 (2024): e231.
|
| [11] |
W. Lu, R. Wang, M. Si, et al., “Synergistic Fluorescent Hydrogel Actuators With Selective Spatial Shape/Color-Changing Behaviors via Interfacial Supramolecular Assembly,” SmartMat 5, no. 2 (2024): e1190.
|
| [12] |
Z. Yang, X. Yan, B. Xu, Z. Wang, and Y. Wang, “Precisely Writing/Printing Hydrogel Patterns on Polymer Surfaces,” Chemical Engineering Journal 485 (2024): 149851.
|
| [13] |
R. Xu, Y. Zhang, S. Ma, et al., “A Universal Strategy for Growing a Tenacious Hydrogel Coating From a Sticky Initiation Layer,” Advanced Materials 34, no. 11 (2022): 2108889.
|
| [14] |
Z. Yang, Y. He, S. Liao, Y. Ma, X. Tao, and Y. Wang, “Renatured Hydrogel Painting,” Science Advances 7, no. 23 (2021): eabf9117.
|
| [15] |
X. Yao, S. Zhang, N. Wei, et al., “Poly(Ionic Liquid) Functionalization: A General Strategy for Strong, Tough, Ionic Conductive, and Multifunctional Polysaccharide Hydrogels Toward Sensors,” SusMat 4, no. 6 (2024): e249.
|
| [16] |
Y. Xue, X. Chen, F. Wang, J. Lin, and J. Liu, “Mechanically-Compliant Bioelectronic Interfaces Through Fatigue-Resistant Conducting Polymer Hydrogel Coating,” Advanced Materials 35, no. 40 (2023): 2304095.
|
| [17] |
J. Wang, X.-Y. Li, H.-L. Qian, et al., “Robust, Sprayable, and Multifunctional Hydrogel Coating Through a Polycation Reinforced (PCR) Surface Bridging Strategy,” Advanced Materials 36, no. 15 (2024): 2310216.
|
| [18] |
J. P. Gong, Y. Katsuyama, T. Kurokawa, and Y. Osada, “Double-Network Hydrogels With Extremely High Mechanical Strength,” Advanced Materials 15, no. 14 (2003): 1155–1158.
|
| [19] |
Y. Zhou, D. Zhang, S. Zhang, et al., “Highly Stretchable Double-Network Gel Electrolytes Integrated With Textile Electrodes for Wearable Thermo-Electrochemical Cells,” SusMat 4, no. 4 (2024): e225.
|
| [20] |
J. W. Hong, H. H. Rana, J. H. Park, et al., “High Na-Ion Conductivity and Mechanical Integrity of Anion-Exchanged Polymeric Hydrogel Electrolytes for Flexible Sodium Ion Hybrid Energy Storage,” SusMat 4, no. 1 (2024): 140–153.
|
| [21] |
J. Steck, J. Kim, Y. Kutsovsky, and Z. Suo, “Multiscale Stress Deconcentration Amplifies Fatigue Resistance of Rubber,” Nature 624, no. 7991 (2023): 303–308.
|
| [22] |
T. Yuan, X. Cui, X. Liu, X. Qu, and J. Sun, “Highly Tough, Stretchable, Self-Healing, and Recyclable Hydrogels Reinforced by In Situ-Formed Polyelectrolyte Complex Nanoparticles,” Macromolecules 52, no. 8 (2019): 3141–3149.
|
| [23] |
J. Yin, N. Liu, P. Jia, et al., “MXene-Enhanced Environmentally Stable Organohydrogel Ionic Diode Toward Harvesting Ultralow-Frequency Mechanical Energy and Moisture Energy,” SusMat 3 (2023): 859–876.
|
| [24] |
Z. Xu, H. Chen, H.-B. Yang, et al., “Hierarchically Aligned Heterogeneous Core-Sheath Hydrogels,” Nature Communications 16, no. 1 (2025): 400.
|
| [25] |
Z. Zhao, Z. Cao, Z. Wu, et al., “Bicontinuous Vitrimer Heterogels With Wide-Span Switchable Stiffness-Gated Iontronic Coordination,” Science Advances 10, no. 10 (2024): eadl2737.
|
| [26] |
T. Long, Y. Li, X. Fang, and J. Sun, “Salt-Mediated Polyampholyte Hydrogels With High Mechanical Strength, Excellent Self-Healing Property, and Satisfactory Electrical Conductivity,” Advanced Functional Materials 28, no. 44 (2018): 1804416.
|
| [27] |
A. P. Liu, E. A. Appel, P. D. Ashby, et al., “The Living Interface Between Synthetic Biology and Biomaterial Design,” Nature Materials 21, no. 4 (2022): 390–397.
|
| [28] |
M. Puertas-Bartolomé, I. Gutiérrez-Urrutia, L. L. Teruel-Enrico, et al., “Self-Lubricating, Living Contact Lenses,” Advanced Materials 36, no. 27 (2024): 2313848.
|
| [29] |
X. Zhang, Y. Liang, S. Huang, and B. Guo, “Chitosan-Based Self-Healing Hydrogel Dressing for Wound Healing,” Advances in Colloid and Interface Science 332 (2024): 103267.
|
| [30] |
A. G. Kurian, R. K. Singh, V. Sagar, J. Lee, and H. Kim, “Nanozyme-Engineered Hydrogels for Anti-Inflammation and Skin Regeneration,” Nano-Micro Letters 16 (2024): 110.
|
| [31] |
Y. Chu, S. Liao, Q. Wang, Y. Ma, and Y. Wang, “Floating Hydrogel Beads Made by Droplet Impact,” Small 18, no. 33 (2022): 2203355.
|
| [32] |
Y. Zhou, M. Cui, S. Liao, et al., “An Injectable Macroporous Hydrogel Templated by Gasification Reaction for Enhanced Tissue Regeneration,” Supramolecular Materials 2 (2023): 100037.
|
| [33] |
X. Wei, S. Fu, and H. Li, “Single-Cell Stereo-Seq Reveals Induced Progenitor Cells Involved in Axolotl Brain Regeneration,” Science 377, no. 6610 (2022): eabp9444.
|
| [34] |
Y. Hua, W. Xu, T. Ye, H. Cai, B. Yin, and H. Wang, “Limb Regeneration Exhibit Both Deterministic and Stochastic Patterns,” Innovation Life 1, no. 3 (2023): 100033.
|
| [35] |
A. Ohashi, H. Sakamoto, J. Kuroda, et al., “Keratinocyte-Driven Dermal Collagen Formation in the Axolotl Skin,” Nature Communications 16, no. 1 (2025): 1757.
|
| [36] |
L. Chen, K. Shi, N. Ditzel, et al., “KIAA1199 Deficiency Enhances Skeletal Stem Cell Differentiation to Osteoblasts and Promotes Bone Regeneration,” Nature Communications 14, no. 1 (2023): 2016.
|
| [37] |
Y. Tian, P. Zhang, Z. Ma, et al., “Single Stem Cell Encapsulation by MnO2 Doped Hydrogel for Robust Bone Regeneration,” Chemical Engineering Journal 513 (2025): 162893.
|
| [38] |
M. Qu, H. Liu, C. Yan, et al., “Layered Hydrogel With Controllable Surface Dissociation for Durable Lubrication,” Chemistry of Materials 32, no. 18 (2020): 7805–7813.
|
| [39] |
X. Xiong, H. Wang, L. Xue, and J. Cui, “Self-Growing Organic Materials,” Angewandte Chemie International Edition 62, no. 47 (2023): e202306565.
|
| [40] |
G. Chen, Y. Yu, X. Wu, G. Wang, J. Ren, and Y. Zhao, “Bioinspired Multifunctional Hybrid Hydrogel Promotes Wound Healing,” Advanced Functional Materials 28, no. 33 (2018): 1801386.
|
| [41] |
Z. J. Wang, J. Lin, T. Nakajima, and J. P. Gong, “Hydrogel Morphogenesis Induced by Force-Controlled Growth,” Proceedings of the National Academy of Sciences of the United States of America 121, no. 27 (2024): e2402587121.
|
| [42] |
D. Mijaljica, F. Spada, D. J. Klionsky, and I. P. Harrison, “Autophagy Is the Key to Making Chronic Wounds Acute in Skin Wound Healing,” Autophagy 19, no. 9 (2023): 2578–2584.
|
| [43] |
S. Roy and S. Gatien, “Regeneration in Axolotls: A Model to Aim for!,” Experimental Gerontology 43, no. 11 (2008): 968–973.
|
| [44] |
W. A. Vieira, K. M. Wells, and C. D. McCusker, “Advancements to the Axolotl Model for Regeneration and Aging,” Gerontology 66, no. 3 (2020): 212–222.
|
| [45] |
W. Han, X.-Q. Xu, X. Lian, Y. Chu, and Y. Wang, “A Degradable Quaternary Ammonium-Based Pesticide Safe for Humans,” CCS Chemistry 6, no. 6 (2024): 1499–1511.
|
| [46] |
S. Zhang, X. Xu, S. Liao, Q. Pan, X. Ma, and Y. Wang, “Controllable Degradation of Polyurethane Thermosets With Silaketal Linkages in Response to Weak Acid,” ACS Macro Letters 11, no. 7 (2022): 868–874.
|
| [47] |
D. K. Owens and R. C. Wendt, “Estimation of the Surface Free Energy of Polymers,” Journal of Applied Polymer Science 13, no. 8 (1969): 1741–1747.
|
| [48] |
D. H. Kaelble, “Dispersion-Polar Surface Tension Properties of Organic Solids,” Journal of Adhesion 2, no. 2 (1970): 66–81.
|
| [49] |
J. Huang, Y. Tang, P. Wang, et al., “One-Pot Construction of Articular Cartilage-Like Hydrogel Coating for Durable Aqueous Lubrication,” Advanced Materials 36, no. 19 (2024): 2309141.
|
| [50] |
R. Li, S. Xu, Y. Guo, et al., “Application of Collagen in Bone Regeneration,” Journal of Orthopaedic Translation 50 (2025): 129–143.
|
| [51] |
H. Zhu, J. Zheng, and X. Y. Oh, “Nanoarchitecture-Integrated Hydrogel Systems Toward Therapeutic Applications,” ACS Nano 17, no. 9 (2023): 7953–7978.
|
RIGHTS & PERMISSIONS
2025 The Author(s). SusMat published by Sichuan University and John Wiley & Sons Australia, Ltd.
PDF
