Background: Caffeine, the only licit psychoactive drug available to minors, may have a harmful impact on students' health and adjustment, yet little is known about its use or effects on students, especially from a developmental perspective. Caffeine use in 5th- and 10th-grade students was examined in a cross-sectional design, and relations and potential mediators of caffeine use to depression and anxiety symptoms were investigated. Methods: Children (n = 135) and adolescents (n = 79) completed a measure of naturalistic use of caffeinated and noncaffeinated beverages. Furthermore, daily availability, perceived benefits, and stimulating, psychological, and withdrawal effects of caffeinated and noncaffeinated beverages were assessed. Measures of depression and anxiety were also administered. Results: Fifth and 10th graders used caffeine frequently. Depression was positively related to caffeine use for both cohorts, though mediated by caffeine withdrawal effects. Surprisingly, anxiety was unrelated to use. Fifth graders reported less daily access to caffeine, but more psychological and stimulating effects of caffeine than 10th graders. Conclusions: Although both children and adolescents experience negative caffeine-related outcomes, intake is seemingly not greatly limited in either cohort. In particular, youth appear vulnerable to increased depressive symptoms with increasing caffeine consumption. Implications for school policy regarding students' caffeine use are discussed. (Contains 4 tables.)