There has been a sizable increase in studies of leadership in inter-school collaboration (ISC) over the past years. But few studies have focused on leaders’ concrete behavior in ISC settings. Drawing on the Leadership for Learning (LfL) theory, this research explored ISC leaders’ behaviors and then surmised underlying leadership styles. A mixed-method design was used to collect data from China. The results showed that the behaviors of high-rated leaders partly revealed that they adopted a caring-oriented leadership style, which focused on situations, needs, and concerns of members. The behaviors of low-rated leaders somewhat presented a control-oriented leadership style, which emphasized dominating the operation of the organization. This research adds to the growing knowledge body of research on leadership in ISC. It not only has important implications for future research but also provides useful implications for ISC leaders’ practice and policy-making.