Hydrogen has emerged as a green and sustainable fuel to meet the demand for future global energy. Nowadays the majority of hydrogen is still produced from steam-reformed methane, which is derived from limited fossil resources and greatly increases CO2 emission. Electrocatalytic hydrogen evolution reaction (HER) enabled by renewable electricity holds great promise as a safe, scalable, low-cost, and environmental-friendly pathway for hydrogen production. In this talk, I will summarize and discuss our recent work for the development of interface controlled nanocatalysis for HER, including the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction that significantly modulates the catalytic activities in either acidic or alkaline HER, highly efficient HER electrocatalyst through a self-gating phenomenon induced by Pt single atoms (SAs) anchored ultrathin NiO nanosheets (NiO-Pt) etc.