The electrochemical hydrogen evolution response (HER) successfully produces clear, renewable, and sustainable hydrogen; nevertheless, the event of environment friendly electrocatalysts is required to scale back the excessive vitality barrier of the HER. Herein, we report two wonderful single-atom (SA)/steel–natural framework (MOF) composite electrocatalysts (PtSA-MIL100(Fe) and PtSA-MIL101(Cr)) for HER. The obtained PtSA-MIL100(Fe) and PtSA-MIL101(Cr) electrocatalysts exhibit overpotentials of 60 and 61 mV at 10 mA cm−2, respectively, that are near that of economic Pt/C (38 mV); they exhibit overpotentials of 310 and 288 mV at 200 mA cm−2, respectively, that are corresponding to that of economic Pt/C (270 mV). Theoretical simulations reveal that Pt SAs modulate the digital constructions of the MOFs, resulting in the optimization of the binding energy for H* and important enhancement of the HER exercise. This examine describes a novel technique for making ready fascinating HER electrocatalysts based mostly on the synergy between SAs and MIL-series MOFs. Utilizing MIL-series MOFs to assist SAs may very well be priceless for future catalyst design.