The results of our investigations on the preparation of 3a,8a-dihydroxyindeno[1,2-d]imidazole derivatives via reaction of thiourea, ninhydrin, and alkyl/benzyl chlorides in aqueous ethanol and under convenient conditions is reported. On the other hand, when uanidinium chloride was used instead of thiourea, the reaction mixtures reached with unexpected products; 2,2-dialkoxy-1H-indene-1,3(2H)-diones.