This article aims to describe the inappropriate use of medicines in the Brazilian urban population and to identify associated factors. We conducted a data analysis of a household survey carried out in Brazil in 2013–14. The sampling plan was done by clusters with representativeness of the urban population and large regions of the country, according to gender and age domains. For this analysis, we considered a sample of adults (≥20 years) who reported having chronic non-communicable diseases, medical indication for drug treatment and medicine use (n = 12 283). We evaluated the prevalence of inappropriate use in the domains: non-adherence, inappropriate use behaviour and inadequate care with medicines, all verified in the following groups of independent variables: demographic and socio-economic characteristics, health and pharmaceutical care, health status and use of medicines. Crude and adjusted prevalence ratios were obtained using robust Poisson regression. It was found 46.1% of people having at least one behaviour of inappropriate use of medicines. The worst results were found for the domain of inappropriate use behaviour, a situation of 36.6% of the users, which included unauthorized prescriber, inadequate source of information and indication of the medicines by non-authorized prescribers. The best result was found for the lack of medicines care, informed by only 4.6% of users who kept expired drugs at home. The inappropriate use of medicines was associated with gender (female), region of residence (Northeast), not visiting the doctor regularly or visiting more than one doctor, not having free access to medicines and using of five or more medicines. There was a high prevalence of inappropriate use, which was associated with both individual and health system characteristics pointing out the need to set priorities as for health education and public interventions.