This report deals with a simple and efficient method to develop hybrid carbon nanoparticles (Nps) employing Multi-walled carbon nanotubes (MWCNTs) and Fullerene nps. Fullerene nps were self-assembled via Ultrasonicated Liquid-Liquid Precipitation. Surface treated MWCNTs were entangled with fullerene nps during the process of assembling of the fullerene nps. Fullerene nps are formed by reaction between two solutions, one is the saturated solution which contains dissolved fullerene and other solution is a rough alcohol. This reaction increases the concentration of carbon in the solution and leads to super saturate hence self-assembling into nanoparticles. The obtained hybrid nanoparticles sizes were in the range of 100 nm to 300 nm with entangled mwcnts and were confirmed by characterization using SEM, Raman, UV-Vis, XRD, and DLS.