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A novel series of 1‐benzylquinazoline‐2,4(1H,3H)‐dione derivatives, 6a,b to 11a–e, was designed, synthesized, and evaluated for their anticancer activity against HepG2, HCT‐116, and MCF‐7 cells. Compounds 11b, 11e, and 11c were found to be the most potent derivatives of all tested compounds against the HepG2, HCT‐116, and MCF‐7 cancer cell lines, with GI₅₀ = 9.16 ± 0.8, 5.69 ± 0.4, 5.27 ± 0.2 µM, 9.32 ± 0.9, 6.37 ± 0.7, 5.67 ± 0.5 µM, and 9.39 ± 0.5, 6.87 ± 0.7, 5.80 ± 0.4 µM, respectively. These compounds exhibited nearly the same activity as sorafenib against HepG2 and HCT‐116 cells and a higher activity against MCF‐7 cells (GI₅₀ = 9.18 ± 0.6, 5.47 ± 0.3, and 7.26 ± 0.3 µM, respectively). Also, these compounds displayed a lower activity than doxorubicin against HepG2 cells and a higher activity against HCT‐116 and MCF‐7 cells (GI₅₀ = 7.94 ± 0.6, 8.07 ± 0 …