An efficient synthesis of substituted indolo[1,2-a]quinolines with indole in the reaction with 2-iodobenzaldehyde derivatives in the present of CuI in deep eutectic solvent (N-phenyliminodiacetic acid: choline chloride (2:1 mol ratio)). The synthetic products were obtained in up to 95% yield. Our mechanistic study confirmed that the reaction sequence involved an intermolecular Knoevenagel reaction followed by an intramolecular Ullmann-type coupling reaction.