Hydrogenated diamond-like carbon (H-DLC) is widely used by the industry, but over the past few decades, its mechanical properties have been hindered by oxidation stemming from frictional contact and heat generation. Herein, we propose a solution by establishing a tribosystem that incorporates two-dimensional black phosphorus (BP) nanosheets and H-DLC. Experiments and atomistic simulations reveal that integration of BP nanosheets to the sliding interface not only shields H-DLC from oxygen erosion, but also creates reactive sites for the formation of hydrogenated fullerene-like carbon (FLC:H) via covalent and hydrogen bonding interactions, resulting in significantly reduced friction. These findings provide a novel insight into the atomic-scale evolution of FLC:H and reveal promising prospects for expanding the industrial application of hydrogenated carbon films.