Few researchers have explored family carers’ perspectives of smoking by their family members with mental illness, despite smoking rates remaining high for people with mental illness. In-depth qualitative interviews with twelve South Australian family carers explored their experiences and views of providing care for people with mental illness who smoke. Data were analysed thematically. Around the central theme of the caring role within the context of mental illness and smoking, were three interrelated themes: (1) responsibility; (2) accommodation; and, (3) dissonance. Carers struggled physically, philosophically and emotionally with perceived responsibilities involving their family member’s smoking. They felt isolated and asserted as there was limited support from service providers to assist them. Carers are important agents within the person’s immediate environment who could potentially help them to improve their smoking cessation success. Community services aiming to support smoking cessation support for this population need to incorporate the role of family carers.