The impact of poor diet quality and nutritional inadequacies on mental health and mental illness has recently gained considerable attention in science. As the opinions and experiences of people living with serious mental illness on dietary issues are unknown, we aimed to understand the role of nutrition in a biopsychosocial approach. In total, 28 semi-structured interviews were conducted with people living with serious mental illness (SMI) in Australia, Germany and Austria, and a generic thematic analysis approach was applied. Four positive (positive effects on the body and mind, therapeutic effects in treating somatic illnesses, pleasure and opportunity for self-efficacy) and three negative (impairment related to mental illness and its treatment, perceived stigma and negative effects on the body and mind) implications of diet were identified. A key issue for most of the participants was the mental burden arising from their body weight. This might indicate that negative implications, such as guilt and stigma, were of primary importance for people with SMI when talking about their dietary behavior. In conclusion, diet-related support is urgently needed for people with SMI. However, especially participants from Germany and Austria reported that this is not yet widely available in mental health settings, leading to hopelessness and resignation.