Background: This study aimed to investigate the relationship between road users' attitudes and their travel behaviors, to explore the acceptability of traffic measures for sustainable transport promotion, and to investigate predictors of intention to reduce car use. Method: Using a cross-sectional survey, 381 residents in Adelaide were interviewed via a computer-assisted telephone interviewing system. Descriptive analysis was used to describe demographic, travel behavior, and effectiveness of potential traffic measures. Attitude statements relating to transport use were factor-analyzed into four factors: “sustainable transport benefits awareness,” “traffic problems awareness,” “cycling safety concerns and car use comfort” and “public transport negative emotion.” Scores on these factors were analyzed with Spearman's correlation and logistic regression. Results: In general, “push” measures (e.g. more expensive petrol) were considered less effective than “pull” measures (e.g. cheaper public transport). “Cycling safety concerns and car use comfort” and “public transport negative emotion” factors were positively related to the annual driving distance of the participants. Both “sustainable transport benefits awareness” and “traffic problems awareness factors” were positively associated with the acceptance of measures for sustainable transport promotion. Furthermore, participants who used cars more frequently, had high sores on “cycling safety concerns and car use comfort,” and had a bachelor degree or higher would be less likely to reduce car use. Conclusion: These findings indicate the importance of increasing public awareness of traffic problems and perceived benefits of sustainable transport as a potential strategy to reduce car use.