Alkaline rechargeable microbatteries have attracted considerable and sustained attention in recent years. However, the complicated fabrication process and the limited specific capacitance of electrodes are still key problems for the development of microbatteries. Herein, we develop a simple approach to enhance electrochemical activity of electrodes via rational design of material components. A sulfide synergistic bimetallic electrode composed of Ni-Co layered double hydroxides (NiCo-LDHs) and Co4S3 composites (NiCo-LDHs-S) is prepared by one-step electrodeposition. Thanks to the richer redox couples in NiCo-LDHs-S and high conductivity of Co4S3, the areal capacitance of NiCo-LDHs-S cathode is similar to 5.8 times, similar to 19.7 times and 1.5 times as high as that of electrodes based on cobalt sulfur composites (Co-O-S), nickel sulfur composites (Ni-O-S) and NiCo-LDHs, respectively. A carbon-modified Fe3O4 (Fe3O4@C) anode is prepared to promote electron transfer, leading to an areal capacitance of 207.2 mC cm(-2) at a current density of 2 mA cm(-2). An efficient alkaline rechargeable microbattery using NiCo-LDHs-S as a cathode and Fe3O4@C as an anode is obtained and shows an areal capacitance of 61.7 mC cm(-2) and an energy density of 16.4 mu Wh cm(-2) (1.0 mW cm(-2)).