The two new complexes, namely [NiU2(H2O)2]SO4, (NiU) and [CuU2(H2O)2]SO4, (CuU) [U = 5,6-diamino-1,3-dimethyl-2,4(1H,3H)-pyrimidinedione monohydrate] were synthesized and characterized by elemental analysis, physicochemical, spectroscopic, (UV-visible, IR, ESI-MS, and XRD), thermal analysis and cyclic voltametric techniques. As showed in the data obtained, an octahedral geometry has been assigned for the two complexes. The data proved that the new complexes NiU and CuU have anticancer activities against colon cancer (HCT-116), epithelioid carcinoma (HeLa), and prostate adenocarcinoma (PC3) human cancer cell lines. The apoptotic pathway for both NiU and CuU complexes was via p53 elevation, which can arrest the cell cycle and activate the release of cytochrome c. The HCT-116 cells were treated with either NiU or CuU complexes had increased the production of caspase-9, which can activate the production of caspase-3 that degrades all the proteins in the cell, leading to apoptotic cell death. Consequently, the two complexes have promising anticancer activities.