Hydrogen fuel cells and water electrolyzers hold significant potential for net zero emission and climate change mitigation, but their practical applications are limited by the use of the precious-metal platinum as catalysts. In this study, a one-pot method is developed for the synthesis of PtCox alloys supported on hybrid carbon materials, and it is found that the developed catalysts with reduced Pt loading can act as excellent bifunctional catalysts for both oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). Morphology and composition characterizations indicate uniform dispersion and adjustable composition of PtCox alloys with the particle size of ∼3 nm on the carbon support. Among them, Pt3Co/C achieves the highest ORR performance with a high mass activity of 179.23 A/g and a specific activity of 3.15 A/m2 in acidic condition, and an extremely low overpotential of 47.6 mV at 10 mA/cm2 in alkaline media as a HER catalyst. This study presents a cost-effective approach for the development of high performance PtCox/C catalysts, and confirms their potential application in hydrogen energy technologies.