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Police officers frequently encounter individuals with mental illness in their duties. However, little research examines factors shaping officers’ perceptions of fair and just treatment toward this population. The current study filling the research gap by examining how organizational support, mental illness literacy, and perceived challenges in policing individuals with mental illness influence officers’ procedural justice when encountering individuals with mental illness. Based on survey data from over 800 police officers in metropolitan Taiwan in 2024, structural equation modeling (SEM) analysis shows that greater organizational support enhances mental illness literacy, reduces perceived challenges in policing individuals with mental illness, and ultimately strengthens officers’ procedural justice. The study confirms both a direct link between organizational support and procedural justice, as well as an indirect link through officers’ literacy and perceived challenges. These findings highlight the importance of strengthening internal training, organizational support, and resources within police agencies to improve procedural justice—both directly and by shaping officers’ knowledge and attitudes.