Much research has been conducted to investigate the impact of work environment on academics' job satisfaction. However, little is known about what contributes to academics' job dissatisfaction. Job satisfaction and job dissatisfaction are two distinct entities because a lack of job satisfaction cannot be simply equated with job dissatisfaction. This research investigated the mediating role of academic self-efficacy in the relationship between perceived work environment and job dissatisfaction. Participants were 547 academics from the 8 University Grants Committee-funded higher educational institutions in Hong Kong. Results show that academics' perceptions of their work environment (including their perceptions of institutional expectations regarding research, university governance and management, and working conditions) statistically predicted job dissatisfaction both directly and indirectly through academic self-efficacy in research and teaching, irrespective of age, gender, academic rank, institutional ranking, and primary academic discipline. The findings enrich the literature concerning perceived work environment, academic self-efficacy, and job dissatisfaction. At the same time, they establish a meaningful link among the fields of psychology, higher education, and career development and have practical implications for academics and university senior managers and, most likely, for senior leaders in other occupations.