Using the micro data of the China Labor Force Dynamics Survey (CLDS), this study constructed an employment quality index of migrant workers by using the factor analysis method, it used the binary logistic model and the intermediary effect model to explore the urban-settlement intention of 1451 migrant workers in 29 cities in China, and it empirically analyzed the impact and internal mechanism of vocational-skills training on migrant workers’ willingness to settle in urban areas. The results show that (1) there is a significant positive relationship between the vocational-skills training and the migrant workers’ settlement intention. A further analysis showed that the empirical results remain robust after correcting endogeneity bias by using the instrumental variable model; and (2) participating in vocational-skills training can improve the employment quality of migrant workers, which would result in the increase of migrant workers’ willingness to settle in urban areas, and employment quality plays the significant intermediary role in this path. (3) The heterogeneity test results show that participating in vocational-skills training has a larger effect on the willingness to settle in urban areas of older-generation, female, and married migrant workers. Therefore, this paper makes the following suggestions: the government should do a good job of top-level design of vocational-skills training for migrant workers, increase investment in human capital of migrant workers, and improve the employment quality of migrant workers.