Layered double hydroxides have demonstrated great potential for the oxygen evolution reaction, which is a crucial half-reaction of overall water splitting. However, it remains challenging to apply layered double hydroxides in other electrochemical reactions with high efficiency and stability. Herein, we report two-dimensional multifunctional layered double hydroxides derived from metal-organic framework sheet precursors supported by nanoporous gold with high porosity, which exhibit appealing performances toward oxygen/hydrogen evolution reactions, hydrazine oxidation reaction, and overall hydrazine splitting. The as-prepared catalyst only requires an overpotential of 233 mV to reach 10 mA·cm^–2 toward oxygen evolution reaction. The overall hydrazine splitting cell only needs a cell voltage of 0.984 V to deliver 10 mA·cm^–2, which is far more superior than that of the overall water splitting system (1.849 V). The appealing performances of the catalyst can be contributed to the synergistic effect between the metal components of the layered double hydroxides and the supporting effect of the nanoporous gold substrate, which could endow the sample with high surface area and excellent conductivity, resulting in superior activity and stability.