Free radical polymerization technique is the most prevalent form of polymerization from academic and commercial perspectives which is broadly applicable to a wide range of monomers. Versatility of this technique is due to the possibility of using various processes that create the free radicals. Ionizing radiation is one of the most direct and easy tools of generating radicals to initiate polymerization, copolymerization, grafting and cross-linking of vinyl and vinylidene type of monomers. Despite its numerous advantages free radical polymerization has the lack of control neither in the molecular weight and its distribution nor on the architecture of polymers. This deficiency has been overcome by using special chain transfer agents that provide reversible addition-fragmentation chain transfer (RAFT) that allows the synthesis of polymers with precise, predetermined molecular weights with very narrow dispersity. In this paper we review the state-of-the-art of radiation-induced RAFT-mediated polymerization for the synthesis of homo-, block-, graft and crosslinked polymers by showing the potential of this technique for some nanotechnology applications.