Preparing nanoparticles with hierarchical structure is a promising approach to improve the interfacial adhesion between additives and polymer matrix. Herein, we exploited hydrothermal carbon spheres (HCSs) decorated with amino-functionalized UiO-66 (UiO-HCSs) to enhance the mechanical and tribological properties of ultrahigh molecular weight polyethylene (UHMWPE) composites. Experimental analyses of the morphologies and chemical structure indicate the successful growth of Zr-based metal-organic frameworks (MOFs) on the surfaces of HCSs. The comprehensive studies reveal the beneficial effects of mulberry-like UiO-HCSs nanoparticles on the interfacial properties. The transfer of Zr-based materials onto the steel counterpart also contributes to decrease the wear rate of UHMWPE composites. Furthermore, the present work may pave route for applying MOFs to tribology.