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This study examined the relationships among person-organization fit, person-job fit, and service behavior by employees in customer-contacted function. This study also examined mediating mechanisms of social exchange with organization and job involvement. We introduced ASA(attraction-selection-attrition) model to explain the relationship between independent variables and a dependent variable. We also introduced social exchange theory and JD-R model to explain the mediating effect of social exchange with organization and job involvement. To examine hypotheses, we collected the data from 204 flight crews in a large airlines of South Korea. The results of regression analysis showed that flight crews’ person- organization fit and person-job fit were positively related to flight crews’ service behavior. The results also showed that flight crews’ person-organization fit was positively related to their social exchange with organization, and that flight crews’ person-job fit was positively related to their job involvement. Finally, the results also showed that flight crews’ social exchange with organization and job involvement were positively related to their service behavior. Consequently, two variables of flight crews’ fit were not only directly related to service behavior, but also indirectly related to service behavior through social exchange with organization and job involvement respectively. This study found the positive relationships among customer-contacted employees’ person-organization fit, person-job fit, and service behavior in service firms. This results showed the importance of cultural and psychological control system to customer-contacted employees in service firms. This study also found the mediating effects of social exchange with organization and job involvement to the relationships among person-organization fit, person-job fit, and service behavior. This results showed the mediating mechanisms for the relationship between person-environment fits and service behavior. We also discussed limitations and further research directions.