The purpose of the study was to synthesize new series of 5-cyano substituted pyrimidine analogues with different substitutions at N1 and 6 positions and to evaluate them for antibacterial and antifungal activities. The desired compounds were synthesized by tertiary condensation of ethylcyanoacetate, substituted thioureas and suitable aldehyde in presence of potassium carbonate using MORE technique. The antibacterial and antifungal activities were evaluated by cup plate method in the concentration of 25 $\mu$g. The zone of inhibition was measured in mm. All the compounds have shown significant antibacterial and antifungal activities. The maximum activity was shown by P1 and P5 against Saureus and E coli respectively, while P6 has shown significant activity against all types of microorganisms. The compound P8 has been found to be significantly effective against C albicans. Norfloxacin and griseofulvin were used as standards to compare the activites of synthesized compounds. It is concluded that analogues containing p-hydroxy, p-methoxy substituted phenyl moiety at 6 position have been found to be more potent against grain-positive microorganisms, while analogues lacking these substituents on phenyl moiety possessed gram-negative activity. The compounds having p-dimethylamino substituent on phenyl moiety at 6 positions have shown moderate activity. Further, only fluorine containing analogue at N1 position was found to possess appreciable antifungal activity. This suggests that electron donating substituent on aryl moiety as well as electron withdrawing substituent at N1 plays important role in determining potency of the compounds.