There is substantial evidence that involuntary job loss can have major implications for workers’ well-being. Yet research on coping with unemployment has most often focused on the job search process and progress toward re-employment, with less emphasis on the process of coping with the myriad psychological challenges of job loss. This study adapted the social cognitive model of career self-management as a framework for understanding well-being and psychological distress during unemployment. Participants were 602 unemployed workers who completed social cognitive measures representing two coping sub-domains, job searching and psychological coping. Within each sub-domain, measures included coping behaviors, self-efficacy, and support. Measures of proactive personality, financial strain, and two psychological functioning criteria (emotional well-being and distress) were also completed. The findings provided initial psychometric support for a novel measure of psychological coping self-efficacy and suggested the utility of the psychological coping variables as predictors of well-being and distress above and beyond job search coping in the context of unemployment. The study’s implications for practice and future research on coping with unemployment are discussed.