A highly efficient, eco‐friendly, recyclable heterogeneous ZnFe2O4 nanocatalyzed synthesis of 2‐amino‐4‐substituted 1,4‐dihydrobenzo[4,5]imidazo[1,2‐a]pyrimidine‐3‐carbonitrile (4a‐j) derivatives via one pot multicomponent reaction of benzimidazole (1), substituted aromatic aldehyde (2a‐j) and malononitrile (3) under ultrasonic irradiations. Significance of this synthetic approach is short reaction time, easy handling, simplicity, efficiency, high yield, and recoverable catalyst.