Purpose: This study aims to determine if neighbourhood psychosocial characteristics contribute to inequalities in smoking among residents from neighbourhoods of differing socioeconomic disadvantage. Methods: This cross-sectional study includes 11,035 residents from 200 neighbourhoods in Brisbane, Australia in 2007. Self-reported measures were obtained for smoking and neighbourhood psychosocial characteristics (perceptions of incivilities, crime and safety, and social cohesion). Neighbourhood socioeconomic disadvantage was measured using a census-derived index. Data were analysed using multilevel logistic regression random intercept models. Results: Smoking was associated with neighbourhood disadvantage; this relationship remained after adjustment for individual-level socioeconomic position. Area-level perceptions of crime and safety and social cohesion were not independently associated with smoking, and did not explain the higher prevalence of smoking in disadvantaged areas; however, perceptions of incivilities showed an independent effect. Conclusions: Some neighbourhood psychosocial characteristics seem to contribute to the higher rates of smoking in disadvantaged areas.