An individual's motivational orientation serves as a drive to action and can influence their career success. This study examines how goal orientation toward the pursuit of a graduate degree in physics and chemistry influences later success outcomes of practicing physicists and chemists. Two main categories of goal orientation are examined in this paper: "performance" orientation or motivation to demonstrate one's ability or performance to others, and "learning" orientation or motivation through the desire to learn about a topic. The data were obtained as part of Project Crossover, a mixed-methods study which focused on studying the transition from graduate student to scientist in the physical sciences and included a survey of members of two national professional physical science organizations. Using regression analysis on data from 2353 physicists and chemists, results indicate that physicists and chemists who reported a "learning" orientation as their motivation for going to graduate school were more productive, in terms of total career primary and/or first-author publications and grant funding, than those reporting a "performance" orientation. Furthermore, given equal salary, "learning"-oriented individuals produced more primary and/or first-author publications than their nonlearning oriented counterparts. (Contains 2 tables and 2 figures.) [A 36-item list of references and notes is provided.]