2D@0D multidimensional nanoparticles (WC@TDP) were first prepared by decorating WS 2 2D nanosheets (WC) with titanium diphenylphosphonate (TDP) 0D nanoparticles, which were derived from the hybridization of diphenylphosphinic acid and TiO 2 . The chemical structure and micromorphology of the modified 2D nanosheet were confirmed, and TDP nanoparticles were tightly attached to the exfoliated WC nanosheets through noncovalent interactions. Afterward, WC@TDP was incorporated into the epoxy resin (EP), showing the improved dispersion and distribution in the thermosetting matrix. Because TDP exhibits catalytic charring activity and WC acts as a physical barrier, such EP/ WC@TDP nanocomposites exhibited the enhanced fire safety, including flame retardation and smoke suppression during burning. The composite containing 8 wt % WC@TDP passed UL94 V-0 rating with a limiting oxygen index increased from 26.0 to 34.0 vol %. Compared with those of neat EP, the peak heat release rate, total heat release rate, and total smoke release of EP/8WC@TDP were reduced by 42%, 17%, and 38%, respectively, without sacrificing the mechanical properties of the nanocomposites.