The study objectives were to characterise the smoking status and quit smoking behaviour of Aboriginal Health Workers (AHWs) in South Australia (SA), Australia; and identify the psychosocial, socio-demographic, and household smoking characteristics that distinguish smokers from quitters and never smokers. A self-reported cross-sectional survey was completed by AHWs in SA. Non-parametric statistics were used for inferential analyses. Eighty-five AHWs completed surveys representing a response rate of 63.0%. The prevalence of current smokers was 50.6%. Non-smokers (49.5%) included quitters (22.4%) and never smokers (27.1%). Smoking status did not differ by gender or geographic location. Of current smokers, 69.0% demonstrated a readiness to quit and 50.0% had made at least one quit attempt in the last 12 months. Compared to quitters and never smokers, current smokers expressed lower emotional wellbeing, and three times as many resided with another smoker. Quitters had the highest levels of perceived social support and part-time employment. A high proportion of AHWs who smoke desire, and are ready to quit. Individual, social and household factors differentiated smokers from non-smokers and quitters. Social support, and relationships and structures that favour social support, are implicated as necessary to enable AHWs who smoke to act on their desire to quit smoking.