There are only a few studies about the effects of toothpastes for children on remineralization and surface roughness of primary teeth. The aim of this study was to examine the remineralization capacity of five different toothpastes for children on primary tooth enamels with artificial initial caries, their effects on enamel surface roughness, and the relationship between their abrasive effects and remineralization. Sixty of 74 samples were allocated for microhardness and AFM analyses (after initialization, demineralization, and pH cycling), and 14 samples were evaluated by SEM. Sixty samples were divided into five groups, with each group representing a different toothpaste brand, as follows: Group 1: Splat; Group 2: Logodent; Group 3: Eyup Sabri Tuncer; Group 4: Naturalive; and Group 5: Buccotherm. Fourteen samples were divided into seven groups, each representing a different processing stage, with two samples in each group, for the initial (sound enamel surface) stage, post demineralization, and after applying the five remineralizing toothpastes. Toothpastes were applied to samples in a 7-day pH cycle. Data were analyzed statistically. Each toothpaste showed increased microhardness values; however, this increase was significant only for Group 4 (Naturalive) and Group 5 (Buccotherm). The highest surface roughness values were obtained after demineralization. The toothpastes reduced surface roughness, but these reductions were not statistically significant among the different types of toothpastes. The correlation analysis revealed that the toothpastes affected surface roughness according to their remineralization potential. The results were supported by SEM images. All toothpastes recovered primary tooth enamels with artificial initial caries, but only two had significant values.