Interface design is a promising strategy for electrocatalysis to optimize charge transfer ability and active sites of a catalyst. Herein, interfacially coupled vanadium telluride and zinc iron telluride nanosheets are synthesized on nickel foam (VTe2@ZnFeTe/NF) by a facile hydrothermal method, which furnishes low overpotentials of 119/217 mV for the hydrogen evolution reaction (HER) and 240/300 mV for the oxygen evolution reaction (OER) at 20/50 mA cm−2 in potassium hydroxide. The alkaline and urea electrolyzer formed by VTe2@ZnFeTe/NF requires an operating voltage of 1.58 V and 1.46 V to yield a current density of 10 mA cm−2 respectively. Density functional theory analysis reveals that the superb activity of VTe2@ZnFeTe/NF is related to its optimal adsorption free energy, extended electroactive centers, excellent charge transfer ability, and reasonable density of states near the Fermi level. These findings provide new insights for the design of transition metal telluride heterointerfaces as catalysts for water and urea electrolyzers.