Coordination across healthcare system levels is a global imperative to ensure efficient resource utilization and provide high-quality care. The substantial body of research on coordination in healthcare mainly concerns coordination across professional and organizational domains. Consequently, there is a dearth of empirical research aimed at delineating the determinants of coordination across healthcare system levels. This paper describes and analyses the barriers and enablers of healthcare coordination across national, regional, and local system levels in a populous Swedish region. Individual interviews and focus group discussions, encompassing a total of 63 individuals, were conducted with managers, administrators, and politicians. The findings of the paper underscore that the barriers identified were most often of a structural or institutional character, whereas the enablers of the studied cross-level coordination were mostly relational. Therefore, we propose that future research should aim to further delineate the prerequisites for personal relationships to emerge, as well as how they may act as enablers of coordination across healthcare system levels.