This study adapted and validated Barnard's Online Self-Regulated Learning Questionnaire (OSLQ) to assess adult learners' (n = 1302) online self-regulation, and examined its relation with attitude towards online learning and perceived online learning satisfaction. It was found that age and employment status were important demographic factors influencing adult learners' online self-regulation. Specifically, middle- and late-career learners perceived themselves to be more self-regulated than early career learners, and self-employed learners perceived themselves to be more self-regulated than out-of-labour learners. Hierarchical regression analysis showed that online self-regulation contributed to adult learners' perceived online learning satisfaction over and above attitude towards online learning and demographic variables. This suggests that online self-regulation is an important predictor of adult learners' online learning satisfaction. Further, within the subscales of online self-regulation, it was found that the more participants set goals and sought help while learning online, the more satisfied they perceived their online learning. Implications for supporting adult learners' online self-regulation and online learning were discussed.