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Background: This study aimed to compare the remineralization effects of sodium caseinate and other substances on artificially demineralized enamel. Methods: We selected 25 healthy human premolars and molars and produced a total of 75 specimens by dividing them into five groups: control group, with distilled water; experimental group 1 (EG1), with 3% sodium caseinate; EG2, with 10% sodium caseinate; EG3, with casein phosphopeptide–amorphous calcium phosphate (CPP-ACP); and EG4, with 0.05% NaF. Subsequently, the specimens were immersed in an artificial demineralization solution for 60 min. The demineralized specimens were then immersed in a remineralization solution for 7 days. Surface microhardness was measured using a microhardness tester, and remineralized lesions were observed under a scanning electron microscope (SEM). Regarding statistical analysis, the paired t-test and analysis of variance were performed using the SPSS program. Results: Although the surface hardness of the remineralized lesions increased significantly in all groups (p <0.05), the average increment did not differ significantly between the groups. The surface microhardness of CPP-ACP was the highest, followed by that of 0.05% NaF and 10% sodium caseinate. The remineralization effect of sodium caseinate was similar to that of 0.05% NaF. SEM confirmed that all groups treated with the remineralization solution were remineralized. Conclusions: Although the remineralization effect of sodium caseinate was slightly lower than that of CPP-ACP, it was similar to that of 0.05% NaF. Therefore, to enhance the remineralization effect of sodium caseinate, the appropriate concentration and application time should be determined.