Novel pyrenyl-moieties-decorated hyperbranched polyglycidol (pHBP) is synthesized and utilized for the functionalization of carbon nanotubes (CNTs) via a non-covalent (non-destructive) process. Mediated by a pHBP layer on the CNT sidewall, Au, Ag and Pt nanoparticles and uniform SiO2, GeO2 and TiO2 coatings are generated in situ and deposited onto the as-prepared CNT/pHBP hybrids, forming versatile homogeneous CNT-based nanohybrid sols. The coverage of metal nanoparticles and oxide coatings is controllable simply by changing the employed amount of precursors. This easy synthetic strategy provides a general and convenient route to efficiently assemble a wide range of metal nanoparticles and inorganic oxide components on the sidewalls of CNTs, and enables the construction of heterogeneous nanostructures with novel functionalities. As a means of demonstrating the versatility of the fabricated hybrid materials, the catalytic function of CNT/pHBP/Pt hybrids towards the reduction of 4-nitrophenol and the incorporation of dye molecules into the CNT/pHBP/SiO2 matrix resulting in fluorescent nanofibers are investigated.