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People living with cancer (PLWC) often face profound existential distress that is insufficiently addressed by conventional psychosocial supports. This qualitative study explored PLWC's attitudes, beliefs, and experiences regarding psychedelic-assisted therapy (PAT) as a novel approach to addressing psychosocial suffering, particularly existential distress. Fifteen participants with varying cancer types and stages were recruited from a national survey. Semi-structured interviews were analyzed using reflexive thematic analysis informed by the Theory of Planned Behavior. Four key themes were identified: (1) Cautious Optimism and Substance-Specific Attitudes Toward Psychedelics reflected varied knowledge, openness, and perceptions of specific agents; (2) Relational and Societal Influences: Stigma, Support, and Cultural Framing; (3) Structural and Systemic Barriers: Cost, Legality, Provider Attitudes, and Unequal Access; and (4) Cancer Context and Psychosocial Needs: Seeking Relief from Existential and Emotional Distress captured the emotional, spiritual, and existential dimensions of living with and beyond cancer. Participants expressed cautious optimism about PAT, driven by unmet needs in conventional care, particularly after active treatment and at advanced stages of cancer, where existential and spiritual concerns often go unaddressed. PAT was seen as a potential adjunct that could meaningfully engage with suffering beyond symptom management. However, concerns about safety, access, and stigma underscore the need for culturally responsive, patient-informed, and equity-focused implementation strategies. Integrating PAT into oncology will require dismantling structural barriers and shifting toward a model of care that embraces the full human experience of serious illness.