This review highlights recent research on the preparation of functional polymeric nanomaterials (nanoparticles, microcapsules, nanofibers, carbon nanotubes) by combined ‘click chemistry’ and controlled radical polymerization (CRP) techniques. In particular, it focuses primarily on combined atom transfer radical polymerization (ATRP), reversible addition-fragmentation transfer polymerization (RAFT), nitroxide-mediated polymerization (NMP), copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) and thiol-ene chemistry. These versatile techniques of polymer synthesis allow the preparation of functional polymeric nanomaterials with well-defined nanostructures and desired functionalities.