2‐Amino‐4‐(4‐substitutedphenyl)‐5‐oxo‐4H,5H‐pyrano[2,3‐d]pyrido[1,2‐a]pyrimidine‐3‐carbonitrile‐derivatives 2–12 were synthesized via multi‐component condensation reactions of different aromatic aldehydes, 3H‐pyrido[1,2‐a]pyrimidine‐2,4‐dione 1, and malononitrile by using ZnO nanoparticles as green chemistry, environmentally friendly catalyst under solvent‐free conditions. The present work creates a variety of biologically active heterocyclic compounds in excellent yield and a short time. The structures of all synthesized compounds were elucidated with the elemental analyses, IR, 1H NMR, and mass spectral data.