High-efficiency electrocatalytic hydrogen evolution reaction (HER) is among the promising approaches for future low-cost hydrogen production. The cost and effectiveness challenges of electrocatalysts have significantly limited the development of electrochemical HER. Metal− organic framework (MOF) derivatives with tunable conformations and remarkable activity have shown unique capabilities in electrocatalytic hydrogen precipitation. Herein, we report a simple method for the synthesis of MOF-derived MoO 2 /NC with decorated Pt nanostructures. Thus, the synthesized MoO 2 /NC/Pt-20 nanostructures with a rod-like structure exhibit better pH-universal HER performance with overpotentials of 32, 53, and 70 mV in alkaline, acidic, and neutral conditions (10 mA• cm −2 ), respectively. Also, the electrocatalysts show low cell voltages of 1.58, 1.59, and 1.70 V at 10 mA•cm −2 for overall water splitting in alkaline, acidic, and neutral conditions, respectively. This research has opened further thought for the rationale for the design of electrocatalysts with stable HER and overall water-splitting performance at all-pH values.