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Due to the critical role of science, technology, engineering, and mathematics (STEM) fields in the nation’s economy and defense, this study aims to explore the factors affecting students’ intentions to pursue STEM careers. Using social cognitive career theory (SCCT) as a framework, we examined the extent to which high school students’ advanced course-taking behavior, mathematics achievement, and motivational beliefs for mathematics and science predicted their plans to pursue STEM careers four years after high school graduation. A nationally representative, large-scale data set—the High School Longitudinal Study 2009 (HSLS:09) was used to conduct binary logistic and hierarchical regression analyses. Results indicated that taking AP mathematics courses and mathematics achievement scores were the strongest predictors of intentions to persist in STEM.