Tetrabutylammonium glycinate [TBA][Gly] ionic liquid was found to be an efficient recyclable and biodegradable organocatalyst for selective synthesis of 3-substituted indoles and indolyl-4H-chromenes. The reaction between substituted aliphatic/aromatic aldehydes, malononitrile, and indoles in the presence of [TBA][Gly] IL at 60 °C under solvent free conditions afforded 3-substituted indoles in excellent yields. Indolyl-4H-chromenes were achieved in excellent yields by replacing the benzaldehydes with salicylaldehyde under optimized reaction conditions.