Squaric acid, a green, metal-free and eco-friendly organocatalyst, has been exploited for the synthesis of biologically interesting 2,3-dihydro-1H-perimidines. The reaction was performed using water as a green reaction medium and the organocatalyst can be easily recovered and reused up to four consecutivecycles without much decrease in catalytic activity. Several advantages of the present methodology are low catalyst loading, excellent catalytic performance, easy catalyst handling, mild reaction conditions, operational simplicity, ease of product isolation, avoidance of column chromatographic separation, a higher yield of the desired product in short reaction time, high atom economy and synthesis of benzophenone based perimidine