Synthesis of fluorescent polyolefins has attracted chemists' considerable attention. While the main methods are based on copolymerization using polar olefins containing fluorophores, the direct synthesis of covalently fluorescent polymers from readily available nonpolar polyolefins is very rare. Herein, we report an efficient protocol for the synthesis of fluorescent polyethylene materials via photoinduced iron catalysis through C−H bond functionalization of polyethylene. Aggregation-induced emission fluorophores, including tetraphenylethylene and benzo[c][1,2,5]thiadiazol-4-yl-triarylamine moieties, could be incorporated to yield fluorescent materials with diverse luminescence between 490 and 650 nm. While these polymers emit in both solid and solution states, a stretchable white light film could be prepared by the blending of three fluorescent polymers. Moreover, this strategy could be used for the functionalization of a series of commonly found plastic products. Experiments further revealed potential applications of these fluorescent polymers as fluorescent compatibilizers and polymeric detectors of nitroaromatic compounds.