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Abstract: An efficient and environmentally benign synthetic method has been developed for the library synthesis of biologically important multi‐functionalized isoindolo[2, 1‐a]quinazolines by two component domino condensation of 2‐carboxybenzaldehyde and 2‐aminobenzohydrazides/2‐aminobenzamides using graphene oxide (GO) as catalyst under solvent free conditions. The solvent‐free strategy exploiting inexpensive and eco‐compatible GO as mild carbocatalyst with large surface area is the major significant advantage of the present protocol. Furthermore, low catalyst loading, good to excellent yield of the products and easy recovery and recyclability of GO attribute considerable supremacy to the present protocol. [ABSTRACT FROM AUTHOR]