5-Benzoy1-6-pheny1-4-(4-mehtoxyphenyI)-1,2,3,4-tetrahydro-2-thioxopyrimidine (1) have been prepared via Biginelli cyclocondensation reaction in acetic acid under reflux condition in good yield. The structure of 1 was determined by using spectroscopic techniques like H-1/C-13 NMR and elemental analyses. And also their molecular characterizations of compounds were analyzed by X-ray crystal analysis. A series of novel pyrimidine derivatives were obtained by reaction compound I with various reactive. All synthesized pyrimidine derivatives and related keto and enol tautomeric forms have been optimized geometrically with DFF in Gaussian at the B3LYP/6-31 + G (d, p) level in order to obtain information about the 3D geometries and electronic structures. The results showed that the keto tautomer is more stable than enol tautomer. However, the non-linear optical (NLO) properties were evaluated theoretically. The electrochemical properties of the novel compounds were investigated by CV and DPV. In addition, the total antioxidant capacities of all new synthesized compounds were measured in vitro by ABTS assay. (C) 2017 Elsevier B.V. All rights reserved.