Governances, structures and contents of mental health services are being reformed across countries. There is a need for data to support those changes. The aim of this study was to explore the quality, i.e., diversity and community orientation, and quantity, i.e., personnel resources, of mental health and substance abuse services (MHS) and evaluate correlation between population needs and quality and quantity of MHS. The European Service Mapping Schedule—Revised (ESMS-R) was used to classify mental health and substance abuse services in southern Finland. Municipal-level aggregate data, local data on unemployment rate, length of education, age of retirement, proportion of single households, alcohol sales and a composite mental health index were used as indicators of population mental health needs. Population size correlated strongly with service diversity, explaining 84% of the variance. Personnel resources did not associate with diversity or community orientation. The indicators of mental health services need did not have the expected association with quality and quantity of services. In terms of service organization, the results may support larger population bases, at least 150,000 adult inhabitants, when aiming for higher diversity.