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Copolymerization provides an effective approach to tune the photophysical properties of non‐conventional luminescent polymers (NCLPs). In this study, the controlling of intrinsic emissions of polyacrylonitrile (PAN) copolymers is revealed by a delicate difference of secondary monomers. The introduction of methacrylate comonomers can induce a 70‐nm red‐shifting in the PL emission of copolymers compared...