A simple one-pot aqueous method is proposed to synthesize PtMo sponge-like nanoporous structure wrapped with ultrathin nitrogen and sulfur co-doped carbon dots by using NaBH₄ as the reductant without any surfactants. The materials are carefully investigated by microscopic (SEM, TEM), spectroscopic (high resolution photoemission, Raman spectroscopy) techniques, evidencing that N,S-co-doped Cdot wraps PtMo sponge-like nanoporous structure. The electrocatalytic activity of the material is tested toward the electrochemical evolution of hydrogen and the electrochemical reduction of oxygen. The obtained N,S-co-doped Cdot/PtMo nanohybrids display enlarged electrochemically active surface area and superior electrocatalytic performances toward hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) in comparison with single PtMo and c-Pt/C catalysts, exhibiting promising applications in energy storage and conversion.