The interaction between host environment and international students plays a critical role in the students' cross-cultural adjustment. However, limited research has captured this interaction in investigating international student acculturation. Building on acculturation and person-environment fit theories, this article investigated student-university alignment of different dimensions as predictors of psychological adjustment of international students at universities in Victoria, Australia. The results of structural equation modeling suggested student-university goal alignment was positively associated with student psychological adjustment. A revealing finding of this article is the mediating role of complementary fit in the relationship between supplementary fit and student psychological adjustment, where the complementary fit was represented by the alignment between student needs and university academic and facilities support, and supplementary fit was represented by student-university goal alignment. The findings have implications for universities and practitioners in developing the necessary resources to support international students.