Herein, the novel core–shell organo-inorganic hybrid carbon nanospheres with encapsulated ultrafine bimetal nanocrystals were successfully prepared by a one-pot domino drive synthesis combined with postcarbonization. The excellent properties of the metals such as high strength and thermal conductivity are retained, and the poor dispersion of the metal in the oil could be improved by encapsulating the metal in organic–inorganic hybrid carbon nanospheres. The vanadium and wolframium nanocrystals embedded in nitrogen-doped carbon nanospheres (V/W@NCNs) manifested remarkable oil dispersity on account of the lipophilic organic phase of the carbon shell. It is worth noting that the as-obtained V/W@NCNs display better tribological properties compared with the base oil, such as a higher extreme pressure of 1250 N, a lower friction coefficient of about 0.09, and a significant reduction in wear volume of 91.5%, which are attributed to the robust protective film that was formed on the surface of the friction pair through mechanical deposition and physical and tribochemical reaction during the friction process.