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Here,we demonstrate that visible light irradiation of trithiocarbonates (TTCs) can effectively induce photo-controlled radical polymerization processes without the aid of any additional radical (photo)initiators or catalysts.This simplistic approach enables the efficient preparation of well-defined,high molecular weight polyacrylates and polyacrylamides with excellent retention of α,ω-end-groups even at high monomer conversions,thus allowing for the efficient formation of (multi)block copolymers of low dispersity in a one-pot fashion.Using the same photo chemistry and RAFT agent,core-crosslinked star (CCS) polymers with high macroinitiator-to-star conversion (> 95%) via a one-pot,two step approach can be achieved.