Graphitic nanoplatelets (GNPs) and luminescent carbon nanoparticles (CNPs) are simultaneously synthesized by controlling the laser parameters and the size of the graphite flakes. Because luminescent CNPs are attached onto GNPs, a new carbon nanostructure is obtained. Compared with carbon black, GNPs, and luminescent CNPs alone, this nanostructure shows better optical-limiting (OL) effects. The OL mechanism of GNPs that are decorated with luminescent CNPs can mainly be attributed to nonlinear scattering. The role of luminescent CNPs is to promote the formation and growth of nonlinear scattering bubbles, thereby enhancing their optical-limiting effects.