Smoking is a major contributor to premature mortality among people with mental illness and substance abuse. Historically, the Substance Abuse and Mental Health Services Administration (SAMHSA) did not include smoking cessation in its mission. We describe the development of a unique partnership between SAMHSA and the University of California, San Francisco’s Smoking Cessation Leadership Center. Starting with an educational summit in Virginia in 2007, it progressed to a jointly sponsored “100 Pioneers for Smoking Cessation” campaign that provided grants and technical assistance to organizations promoting cessation. By 2013, the partnership established 7 “Leadership Academies,” state-level multidisciplinary collaboratives of organizations focused on cessation. This academic–public partnership increased tobacco quit attempts, improved collaboration across multiple agencies, and raised awareness about tobacco use in vulnerable populations.