Background: Research on the co-occurrence of unhealthy lifestyles has tended to focus mainly upon the demographic and socioeconomic characteristics of individuals. This study investigated the relevance of neighborhood socioeconomic circumstance for multiple unhealthy lifestyles. Method: An unhealthy lifestyle index was constructed for 206,457 participants in the 45 and Up Study (2006–2009) by summing binary responses on smoking, alcohol, physical activity and five diet-related variables. Higher scores indicated the co-occurrence of unhealthy lifestyles. Association with self-rated health, quality of life; and risk of psychological distress was investigated using multilevel logistic regression. Association between the unhealthy lifestyle index with neighborhood characteristics (local affluence and geographic remoteness) were assessed using multilevel linear regression, adjusting for individual-level characteristics. Results: Nearly 50% of the sample reported 3 or 4 unhealthy lifestyles. Only 1.5% reported zero unhealthy lifestyles and 0.2% had all eight. Compared to people who scored zero, those who scored 8 (the ‘unhealthiest’ group) were 7 times more likely to rate their health as poor (95%CI 3.6, 13.7), 5 times more likely to report poor quality of life (95%CI 2.6, 10.1), and had a 2.6 times greater risk of psychological distress (95%CI 1.8, 3.7). Higher scores among men decreased with age, whereas a parabolic distribution was observed among women. Neighborhood affluence was independently associated with lower scores on the unhealthy lifestyle index. People on high incomes scored higher on the unhealthy lifestyle index if they were in poorer neighborhoods, while those on low incomes had fewer unhealthy lifestyles if living in more affluent areas. Interpretation: Residents of deprived neighborhoods tend to report more unhealthy lifestyles than their peers in affluent areas, regardless of their individual demographic and socioeconomic characteristics. Future research should investigate the trade-offs of population-level versus geographically targeted multiple lifestyle interventions.