Searching for ideal candidates with high electrocatalytic performance for both HER and OER is a major objective to realize the large-scale H2 production by seawater electrolysis. Herein, we report delicate, heterostructured NiTe-NiCoN and NiTe-NiFeN electrocatalysts, which exhibit outstanding HER and OER performance, respectively. Impressively, the NiTe-NiCoN || NiTe-NiFeN couples in alkaline seawater solution delivered 400 mA cm−2 at 1.84 V along with long-term stability. Further analysis has revealed that not only heterogeneous interface engineering ensures exposure of abundant active site...