A series of 1,6-dihydro-2-hydroxyethylamino-6-oxo-4-arylpyrimidine-5-carbonitriles 8a-i, and 4-amino-2-hydroxyethylamino-6-arylpyrimidine-5-carbonitriles 9a-i were prepared. Multicomponent reaction of araaldehyde 1a-i , S-methylisothiourea sulfate 2 with ethyl cyanoacetate 3 afforded 1,6-dihydro-2-methylthio-6-oxo-4-arylpyrimidine-5-carbonitriles 4a-i. Also, multicomponent reaction of 1, 2 with malononitrile 5 afforded 4-amino-2-methylthio-6-arylpyrimidine-5-carbonitriles 6a-i. Reaction of compounds 4a-i, and 6a-i with ethanolamine 7 under solvent free condition at 130-140 °C afforded 8a-i, and 9a-i respectively. The purity of the new compounds was checked by TLC and elucidation of their structures was confirmed by IR, 1H-NMR, 13C-NMR and HRMS spectrometry. Compounds were subjected to NCI in vitro assessment for their anticancer activity at a single dose of 10 μM of test compounds, Also, all of the tested compounds were in vitro assessment for their antibacterial and antifungal activities in a comparison to chloramphenicol and clotrimazole as reference antibacterial and antifungal drugs respectively. All the tested compounds showed varied anticancer activities ranging from weak to moderate activities. In the other