For doing businesses succeed in today¡¦s competitive environment, Taiwanese companies vary their human resources strategies, such as downsizing, outsourcing or removing production section to lower labor cost region. All of these practices impacted the employees¡¦ job securities. At the same time, the young employees have some different points of view to employment contract. The employment relationship is changing. A psychological contract is an employee's belief about the mutual obligations, and it balances the relationship between the employee and his/her organization. According to the three different types of psychological contact, employees start to think what kind of knowledge they shall learn to benefit both of job availability and career development. The purpose of this study is to examine the relationship among psychological contracts, job availability in free labor market, and employee knowledge learning aspirations. Based on the data from 990 employees from 62 firms analyzing, the researcher obtained the following findings: 1. The difference: a. Gender, educational degree, and job position revealed difference with regard to psychological contract. b. Gender, marriage, age, and job position revealed difference with regard to firm-specific knowledge learning aspiration. c. Age, marriage and job position revealed difference with regard to general knowledge learning aspiration. 2. The relationship: a. Relational and balanced psychological contracts are positively related to firm-specific knowledge learning aspiration. b. Transactional psychological contract has negative relation with firm-specific knowledge learning aspiration. c. Job availability in free labor market is positively related with general knowledge learning aspiration.