This study is original in that it assesses various types of care needs, barriers to care, and factors associated with higher unmet needs among 308 permanent supportive housing (PSH) residents in Quebec (Canada). Data from structured interviews that featured the Perceived Need for Care Questionnaire were collected from 2020 to 2022, controlling for the COVID-19 pandemic period. Eight types of care (e.g., information, counseling) were accounted for. Based on the Behavioral Model for Vulnerable Populations, predisposing, need, and enabling factors associated with higher unmet care needs were assessed using a negative binomial regression model. The study found that 56% of adult PSH residents, even those who had lived in PSH for 5 + years, had unmet care needs. Twice as many unmet needs were due to structural (e.g., care access) rather than motivational barriers. Living in single-site PSH, in healthier neighborhoods, having better quality of life and self-esteem, and being more satisfied with housing and outpatient care were associated with fewer unmet care needs. PSH residents with co-occurring mental disorders (MD)and substance use disorders (SUD), and with moderate or severe psychological distress were likely to have more unmet needs. Better access to care, counseling and integrated treatment for co-occurring MD-SUD might be improved, as well as access to information on user rights, health and available support. Welfare benefits could be increased, with more peer support and meaningful activities, especially in single-site PSH. The quality of the neighborhoods where PSH are located might also be better monitored.