Comprehensive Summary New blue‐light promoted methods for the addition of iodoacetonitrile (ICH2CN) to alkene/alkynes have been developed. The reaction led to the formation of cyanoalkylated products when conjugated alkene/styrene was used. In the case of alkynes and non‐conjugated alkenes, iodoalkylation takes place furnishing the corresponding alkenyl iodides and alkyl iodides, respectively. Notably, trans‐alkenyl iodides were obtained as the major product. A plausible reaction mechanism is also proposed.

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