This study had two objectives. First, responding to calls for improved measurement of outcome expectations in the domain of career exploration and decision-making (Fouad & Guillen, 2006), a measure of outcome expectations was developed that incorporates Bandura’s (1997) conceptualization of both positive and negative outcomes, as well as classes of physical, social, and self-evaluative effects. Second, the replicability of the scale’s factor structure and evidence of its validity were examined. Social cognitive career theory (SCCT; Lent & Brown, 2013) was used to explore the theoretical relationships between positive and negative outcome expectations, and other domain-specific variables, including (a) self-efficacy, (b) learning experiences, (c) social support, and (d) career exploration goals. In addition to exploring direct relationships proposed by the SCCT career self-management model, negative outcome expectations were also explored for their theorized moderation of the relations of self-efficacy to goals and positive outcome expectations to goals. Data were collected via an online survey in two separate samples of college students who were in the process of making initial career decisions. Exploratory and confirmatory factor analyses of the new outcome expectations measure indicated a 22-item, four-factor scale with distinct positive and negative factors. Subsequent measure and hypothesis testing analyses offered support for the convergent and discriminant validity of the scale in the samples, found that exploratory intentions was linked with both self-efficacy and positive outcome expectations, and indicated a potential moderator role for negative outcome expectations in these relationships.