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Despite the well-established need to increase access to HIV testing and prevention services among people with serious mental illness, little is known about the determinants of implementation of these services in behavioral health organizations. This multi-method study was conducted in King County, Washington, an EHE priority jurisdiction. A quantitative survey of 16 county behavioral health organizations explored the HIV testing and prevention services currently offered. Three organizations that viewed HIV testing and prevention services as very important or essential for their clients participated in in-depth qualitative interviews; 21 staff, providers, and leaders were interviewed about barriers and facilitators to on-site HIV testing and prescription or referral for Pre-exposure prophylaxis (PrEP). We used a rapid deductive qualitative analysis approach guided by the Consolidated Framework for Implementation Research (CFIR) 2.0. Commonly identified facilitators were organizational culture and a non-judgmental approach to care, frequent contact and long-standing relationships with clients, and a mission to provide holistic care. Commonly identified barriers were lack of resources and trained staff, infrastructure challenges (inability to bill services, weak referral pathways), higher priorities for services (including testing for Hepatitis C and sexually transmitted infections), and lack of knowledge and information. Lack of trained staff and the complexity of the service were more often perceived as barriers to providing PrEP on-site than HIV testing. Opportunities to build capacity were also identified, and included training, implementing universal testing, and expanding partnerships with other organizations to provide HIV testing and prevention services on-site at the behavioral health organization.