In Australia, the prevalence of smoking is higher among certain sub-populations compared to the general population. These sub-populations include Aboriginal and Torres Strait Islander people, people from culturally and linguistically diverse backgrounds, as well as people with mental and substance use disorders and prisoners. The aims of this paper are to: describe the high prevalence of smoking among these particular sub-populations and harms associated with smoking; explore possible reasons for such high prevalence of smoking; review the evidence regarding the efficacy of existing smoking cessation interventions; and make recommendations for smoking interventions and further research among these groups. In addition to low socio-economic status, limited education and other factors, there are social, systems and psychobiological features associated with the high prevalence of smoking in these sub-groups. General population-based approaches to reducing smoking prevalence have been pursued for decades with great success and should be continued with further developments that aim specifically to affect Aboriginal and Torres Strait Islander people and some cultural groups. However, increasing attention, more specific targeting and flexible goals and interventions are also required for these and other distinct sub-populations with high smoking prevalence. Recommendations include: more funding and increased resources to examine the most appropriate education and treatment strategies to promote smoking cessation among people from Aboriginal and Torres Strait Islander and some culturally and linguistically diverse backgrounds; larger and better-designed studies evaluating smoking cessation/reduction interventions among distinct sub-groups; and system-wide interventions requiring strong leadership among clients and staff within mental health, drug and alcohol and prison settings.