ABSTRACT This study employed components drawn from Social Cognitive Career Theory (SCCT), the person agency and environment, to investigate the determinants of career-relevant knowledge/skills learning. Three types of psychological contract (PC) and self-efficacy (SE) were represented the person agency, and the job availability in free labor market (FLM) and commitment-oriented human resource management (HRM) were represented environment components. Based on the data from 990 employees from 62 firms analyzing, the findings revealed that relational and balanced PCs are positively related to firm-specific knowledge learning aspiration (KLA), whereas transactional one has negative relation with firm-specific KLA. FLM is positively correlated with self value-added KLA. SE is positively related to both KLAs. The three way interaction of relational and balanced PC, FLM, and SE has significant impacts on self value-added KLA. HRM has no direct impact on KLAs , but moderates the relationship between relational/balanced PC and firm-specific KLA. This study contributes to the psychological contract and SCCT researches, and the findings enhance the understanding of employees¡¦ concerns about their learning decisions which assist employer to consider their knowledge management strategy and practices.