context: In this paper, MoP and NiCo-LDH are used to synthesize a composite of MoP@NiCo-LDH, which is supported on nickel foam to form a bifunctional composite catalyst (abbreviated as MoP@NiCo-LDH/NF), as shown in Fig. 1. During the synthesis, different electrodeposition times are used to optimize the catalyst's performance toward both UOR and HER. Both instrumental characterization and electrochemical measurements confirm that the composition between MoP and NiCo-LDH as well as their electrodeposition onto the NF surface can increase the material's specific surface area and produce a synergetic effect toward high performance. To validate this bifunctional catalyst, a two-electrode electrolyser (MoP@NiCo-LDH/NF-20‖MoP@NiCo-LDH/NF-20) with this catalyst on both the anode and the cathode was designed and constructed, and the test results show that this catalyst has better catalytic performance than that of a Pt/C/NF‖IrO2/NF electrolyser, where noble metal materials (Pt and IrO2) are used as the catalysts.