Synthesis of Pyrimidino-4,6-(2,4-Diazepine) derivatives were achieved by green and one pot synthesis using 1,2-diketones and 4,6-diamino Pyrimidines as the precursor of condensation reaction and CTAB as the cationic surfactant. For the purpose of determining the efficiency of substituent on 1,2-diketones, three different forms of diketones were used viz., Benzil, 4,4'-dimethyl Benzil and 4,4'-difluoro Benzil. The results showed that the use of 4,4'-difluoro Benzil, was better among the three Benzils, considering its yield and the time consumption. All the three types of Benzodiazepine derivatives so obtained were independently used for evaluating their anxiolytic, sedative and hypnotic activity using albino mice as the subject. When the resultant Pyrimidino-benzodiazepines was compared with standard Diazepam, the following results were obtained: Sedative and Hypnotic activity >Standard Diazepam, but Anxiolytic activity< Standard Diazepam. In most cases, Fluoro substituted Diazepine show deviation in activity. The results in locomotor activity suggest the appreciable alertness of the mice when exposed to Pyrimidine based Diazepine drugs.