We investigated grit and its relations with students' self-regulated learning (SRL) and academic achievement. An ethnically diverse sample of 213 college students completed an online self-report survey that included the Grit Short scale (Duckworth and Quinn "Journal of Personality Assessment, 91(2)," 166-174, 2009), seven indicators of SRL and their past and present academic achievement. Results indicated that one aspect of grit, perseverance of effort, was a consistent and adaptive predictor for all indicators of SRL including value, self-efficacy, cognitive, metacognitive, motivational, time and study environment management strategies, and procrastination. A second aspect of grit, consistency of interest, was associated only with the latter two facets of SRL. Perseverance of effort predicted achievement before, but not after, accounting for SRL; hence, students' engagement in SRL may serve as a mediating pathway through which this aspect of grit is associated with improved academic outcomes. In contrast, consistency of interest showed no relation to achievement. Implications of the findings for additional research and instruction are discussed.