Individuals diagnosed with serious mental illnesses continue to experience work-related disparities despite the existence of evidence-based practices. Understanding the meaning of work among these individuals is key to developing interventions grounded in career development theory and practice. This qualitative inquiry adapted a consensual qualitative research approach and utilized a participatory component to conduct an in-depth exploration of the meaning of work among a national sample of young adults and older adults living with serious mental illness. The psychology of working perspective was applied to the results after analyses. Results revealed categories that clustered within four overarching domains pertaining to work as central to survival, social connectedness, self-determination, and mental health recovery as proposed by the theory. Implications for services, research, and policy are discussed.