A simple and versatile approach has been developed to synthesize different carbon nanotube (CNT)-nanoparticle hybrid materials. The strategy is based on the nondestructive (noncovalent) functionalization of pristine CNTs and the subsequent in situ synthesis of a variety of different nanoparticles, including metal, semiconductor, and insulator particles, on the modified CNTs. This strategy has been demonstrated here with Pt, US, and silica nanoparticles. It is believe that this technique will provide a simple and convenient route to efficiently assemble a wide variety of nanoscale particles/clusters on the surfaces of CNTs, and will enable the construction of nanoscale heterostructures with novel functionalities in nanotechnology.