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Photo‐iniferter reversible addition‐fragmentation chain transfer (PI‐RAFT) polymerization of N‐vinylformamide (NVF) is demonstrated by using purple light. PNVFs with predetermined molar masses and narrow molar mass distributions are obtained. High RAFT chain‐end fidelity is confirmed by matrix‐assisted laser desorption ionization time‐of‐flight (MALDI‐TOF) and electrospray‐ionization time‐of‐flight...