The development of bifunctional electrocatalysts with efficient oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is still a key challenge at the current stage. Herein, FeNi LDH/V2CTx/nickel foam (NF) self-supported bifunctional electrode was prepared via deposition of FeNi LDH on V2CTx/NF substrate by hydrothermal method. Strong interfacial interaction between V2CTx/NF and FeNi LDH effectively prevented the aggregation of FeNi LDH, thus exposing more catalytic active sites, which improved electrical conductivity of the nanohybrids and structural stability. The results indicated that the prepared FeNi LDH/V2CTx/NF required 222 mV and 151 mV overpotential for OER and HER in 1 M KOH to provide 10 mA cmâ2, respectively. Besides, the FeNi LDH/V2CTx/NF electrocatalysts were applied to overall water splitting, which achieved a current density of 10 mA cmâ2 at 1.74 V. This work provides ideas for improving the electrocatalytic performance of electrocatalysts through simple synthesis strategies, structural adjustment, use of conductive substrates and formation of hierarchical structures.