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Self-regulated learning (SRL) is a multifaceted process integrating both cognitive and motivational elements as learners monitor, regulate, and control the amount of time and effort required to complete tasks and achieve goals. This study used a multilevel cross-classified analysis that nested effects both within participants and weeks with a moderation analysis to disambiguate the relationships among cognitive load, self-efficacy, and goal setting over time using data from university students engaged in an online course. Findings indicate that the main and interaction effects of cognitive load and self-efficacy on goal setting are positive and significant. Implications of these findings suggest that models of SRL are fundamentally incomplete without accounting for the dynamic interactions between cognitive load and self-efficacy.