As the serious economic depression has persisted, the unemployment as well as underemployment has emerged as social and economic issues in recent years. Overqualification, a mode of underemployment, refers to the situation where employees possess higher qualifications than job requirements. In general, scholars have insisted that employees overqualified for their job tend to show negative or counterproductive behaviors. The current research was aimed at exploring the way to mitigate the negative influence of overqualification and to turn it into a positive one. Drawing on career construction theory and person-job fit theory, this research examined the relations among career adaptability, job crafting, perceived overqualification and organizational commitment. First, the result represented the significant mediating effect of job crafting between perceived overqualification and organizational commitment. Second, the moderating impact of career adaptability significantly enhanced the relation between perceived overqualification and job crafting. Third, the moderating impact of career adaptability significantly strengthened the relation between job crafting and organizational commitment. These findings provide meaningful insights into managing the employees’ perception of overqualification and applying the identified roles of job crafting and career adaptability to human resource development.