Objectives: This study evaluated the effect of different nanoparticulated zinc oxide (nanoZnO) and conventional-ZnO ratios on the physicochemical properties of calcium aluminate cement (CAC). Materials and Methods: The conventional-ZnO and nano-ZnO were added to the cement powder in the following proportions: G1 (20% conventional-ZnO), G2 (15% conventionalZnO + 5% nano-ZnO), G3 (12% conventional-ZnO + 3% nano-ZnO) and G4 (10% conventional-ZnO + 5% nano-ZnO). The radiopacity (Rad ), setting time (Set ), dimensional change (Dc ), solubility (Sol ), compressive strength (Cst ), and pH were evaluated. The nanoZnO and CAC containing conventional-ZnO were also assessed using scanning electron microscopy, transmission electron microscopy, and energy-dispersive X-ray spectroscopy.Radiopacity data were analyzed by the 1-way analysis of variance (ANOVA) and Bonferroni tests (p < 0.05). The data of the other properties were analyzed by the ANOVA, Tukey, and Fisher tests (p < 0.05). Results: The nano-ZnO and CAC containing conventional-ZnO powders presented particles with few impurities and nanometric and micrometric sizes, respectively. G1 had the highest R ad mean value (p < 0.05). When compared to G1, groups containing nano-ZnO had a significant reduction in the S et (p < 0.05) and lower values of D c at 24 hours (p < 0.05). The C st was higher for G4, with a significant difference for the other groups (p < 0.05). The S ol did not present significant differences among groups (p > 0.05). Conclusions The addition of nano-ZnO to CAC improved its dimensional change, setting time, and compressive strength, which may be promising for the clinical performance of this cement.