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Novel copper complex based initiating systems for redox free radical polymerization (FRP) of methacrylate resins under mild conditions are proposed. Remarkably, the FRP performance of the Cu( i )/ascorbic acid (Vitamin C – VitC)/benzoyl peroxide (BPO) redox system is noticeably more significant than that of the amine/BPO reference especially at the top surface where the oxygen inhibition is particularly deleterious. The Cu( i )/BPO interaction leads to a decomposition of the peroxide and generates a benzoyl radical and Cu( ii ) as a byproduct. The ascorbic acid acts as a reducing agent and allows the regeneration of Cu( i ) from Cu( ii ). Hydroperoxides formed at the surface through the radical/O 2 interaction are also decomposed by the new proposed Cu complex leading to additional polymerization initiating species. The structure/reactivity relationship of the new proposed Cu( i ) complexes in the Cu( i )/VitC/BPO systems is studied. The use of Cu( i )/VitC/BPO/iodonium salt systems in redox photoactivated FRP is also explored.