Iron homeostasis is important for maintaining normal physiological brain functioning. In two independent samples, we investigate the link between iron concentration in the basal ganglia (BG) and implicit sequence learning (ISL). In Study 1, we used quantitative susceptibility mapping and task-related fMRI to examine associations among regional iron concentration measurements, brain activation, and ISL in younger and older adults. In Study 2, we examined the link between brain iron and ISL using a metric derived from fMRI in an age-homogenous sample of older adults. Three main findings were obtained. First, BG iron concentration was positively related to ISL in both studies. Second, ISL was robust for both younger and older adults, and performance-related activation was found in fronto-striatal regions across both age groups. Third, BG iron was positively linked to task-related BOLD signal in fronto-striatal regions. This is the first study investigating the relationship among brain iron accumulation, functional brain activation, and ISL, and the results suggest that higher brain iron concentration may be linked to better neurocognitive functioning in this particular task.