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The catalyst‐free electrochemical halogenation and trifluoromethylation of 4H‐pyrido[1,2‐a]pyrimidin‐4‐ones was realized under external‐oxidant‐free conditions. This strategy provides an easy and green access to functionalized new 4H‐pyrido[1,2‐a]pyrimidin‐4‐one derivatives with broad scope, good functional group tolerance and high regioselectivity.