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Tobacco use is prevalent among military veterans. Veterans with serious mental illness (SMI) smoke cigarettes at higher rates than their counterparts, which causes major health disparities. Additional efforts are needed to support smoking cessation in this population. This study was informed by the theory of planned behavior and used a rapid qualitative matrix approach to explore how attitudes, perceived behavioral control, and social norms influenced smoking among veterans with SMI to inform tailored treatment. In a sample of 20 veterans, smoking initiation was often linked to military culture and early exposure to smoking. Peer pressure and social belonging either facilitated or inhibited quit attempts. Veterans wanted to quit, but continued smoking due to addiction and to cope with mental health challenges. Smoking cessation discussions for veterans with SMI should be integrated into routine mental health care and explore social norms around smoking, coping strategies, and the psychological benefits of quitting.