A practical and green approach for the ultrasound-enhanced one-pot multicomponent synthesis of tetraheterocyclic imidazo(thiazolo)pyrimidines is described via the condensation of an 2-aminobenzimidazole or 2-aminobenzothiazole, dimedone and various aldehydes in the presence of FeO@clay as an environmentally benign and reusable core/shell nanocomposite catalyst in relatively quantitative yields. This novel eco-friendly protocol includes several advantages such as avoiding hazardous solvents, reusability of the catalyst, easy work-up, short reaction times, room temperature and mild reaction conditions. Furthermore, ultrasonic irradiation and synergistic catalyst showed considerable superiority vs. traditional heating or stirring conditions.