Toothpastes available in Europe contain a range of fluoride concentrations, with some meeting the recommended level for caries prevention (>1000 ppm fluoride (ppm)) and others containing low or no fluoride. This study evaluated toothpaste fluoride concentrations in Latvia and Lithuania to inform targeted public health strategies in regions with a high prevalence of dental caries. This cross-sectional study was conducted from May 2019 to May 2020, using a validated questionnaire in Latvia and Lithuania. Nationally representative samples (1309 families and 5436 members) provided data through a mixed-mode survey (paper and online) on sociodemographic information, toothpaste type, brand, and type. Descriptive statistics and chi-square tests (p < 0.05) were used for analysis. Fifteen percent of families used non-fluoridated toothpaste and 12% used <1000 part per million (ppm) fluoride. In Latvia, 56.8% of preschoolers and 28.7% of schoolchildren used <1000 ppm or non-fluoride toothpaste, whereas in Lithuania, 47.2% of preschoolers and 29.1% of schoolchildren used <1000 ppm or non-fluoride toothpaste; 63% of adolescents and 73% of adults used toothpaste with optimal fluoride content (≥1000 ppm). Of the 228 registered toothpaste types, 62% contained more than 1000 ppm, which is optimal for caries prevention; 29% of Latvian and 24% of Lithuanian families used at least one non-fluoridated toothpaste. This study revealed significant gaps in the use of fluoride toothpaste among families in Latvia and Lithuania, especially among children. To effectively prevent dental caries, targeted interventions, and education must promote optimal fluoride toothpaste use, particularly among vulnerable populations.