Cycling is widely regarded as a healthy and sustainable transport option in urban environments. However, there is an emergent need to understand how cycling in countries like Brazil, can be encouraged and supported, particularly among different sections of the population. This study investigates social-psychological antecedents of cycling within the Brazilian context using a large-scale dataset to verify the appropriateness of a model based on the extended Theory of Planned Behaviour (e-TPB). In-person interviews were conducted with people living in three large Brazilian cities – Brasília (n=1107), Florianópolis (n=1084), and Porto Alegre (n=1105) using a questionnaire including nine items from the e-TPB to measure attitudes, social norms, perceived behavioural control, intention, cycling behaviour, and habit. Multigroup analysis verified the model fit and invariance in structural weights by gender. Age and gender were revealed to be the only sociodemographic variables with significant influence on the components’ mean scores, with gender exhibiting the strongest influence. We concluded that the e-TPB allows us to explain cycling behaviour among this sample of the Brazilian population and that it is particularly sensitive to (a) other people's influence (b) personal habit (c) perceived behavioural control (d) belief in the ability to change one’s behaviour. Women were less likely to cycle and were less likely to be influenced by social-psychological components that could encourage this type of activity. Thus, we conclude that understanding the social and cognitive determinants of cycling can help to design more targeted policies for different sections of society.