There is a strong association between urban prosperity and human resources. Rapid urbanization and industrialization have caused severe air pollution to the urban cities over the past decades, and permanently moving to locations with clean air has been considered to be one of the most effective strategies to avoid air pollution. However, whether this is in fact still unclear. In order to fill the research gaps, this study combines individual-level data derived from a national survey and city-level data obtained from various sources to empirically exam the effect that air quality has on settlement decisions of urban floating migrants in China. We focus on the target floating migrants who have urban hukou in the origin city and housing in the destination city, and investigate the relationship between air quality and settlement decisions from the move-in and move-out city perspective. In addition, we exam not only the willingness of urban floating migrants to settling in the move-in city, but also their actual migration decision in the reality. The bivariate probit analysis and panel data regression are applied. Results show that poor air quality in the move-out cities has a significant positive impact on urban floating migrants’ willingness to settling in the move-in cities, while bad air quality in the move-in cities has a significant negative impact, indicating that poor air quality does act as a push force to drive floating migrants away but good air quality can be a pulling force for floating migrants to settling down. In addition, the robust tests show good agreement with the main regression results, with almost all relationships reported having the same direction as those indicated by the regression analysis. Our findings can help policy makers and urban planners assess and design interventions to improve the urban air quality aimed at attracting talent, with broader implications for urban sustainable development.