Previous studies showed that control beliefs are more strongly related to global cognition and mortality among adults with low education, providing preliminary evidence that self-efficacy buffers against the negative impact of educational disadvantage on physical and cognitive health. The current study extends these findings to a nationally representative sample of men and women aged 30 to 85 and explores which cognitive domains are most strongly associated with self-efficacy, educational attainment, and their interaction. Data were obtained from 1032 adult (30–85) participants in the United States norming study for the NIH Toolbox. Self-efficacy, executive functioning, working memory, processing speed, episodic memory, and vocabulary were assessed with the NIH Toolbox. Multivariate analysis of covariance and follow-up regressions tested the hypothesis that self-efficacy would be more strongly related to cognitive performance among individuals with lower education, controlling for age, sex, race, ethnicity, education, reading level, testing language, and depressive symptoms. Higher education was associated with higher self-efficacy and better performance on all cognitive tests. Higher self-efficacy was associated with better set-switching and attention/inhibition. Significant self-efficacy by education interactions indicated that associations between self-efficacy and executive abilities were stronger for individuals with lower education. Specifically, individuals with low education but high self-efficacy performed similarly to individuals with high education. This study provides evidence that self-efficacy beliefs buffer against the negative effects of low educational attainment on executive functioning. These results have implications for future policy and/or intervention work aimed at reducing the deleterious effects of educational disadvantage on later cognitive health. (JINS, 2015, 21, 297–304)