Aims Investments to promote public transport utilisation are being championed to achieve sustainable development, but the potential co-benefits for mental health are comparatively under-researched. We hypothesised that frequent users of public transport would be more likely to have better mental health (possibly due to increased levels of physical activity), but among the more frequent users, less favourable perceptions of public transport infrastructure (PPTI) could have a negative influence on mental health. Methods Multilevel linear and logistic regressions were fitted on 30,214 participants in the UK Household Longitudinal Study with lagged PPTI and confounder measures at baseline and indicators of active travel and mental health (General Health Questionnaire (GHQ), SF-12 Mental Component Scale (MCS) and the Warwick Edinburgh Mental Well Being Scale (WEMWBS)) at follow-up. Results Compared to participants expressing poor PPTI, those who felt it was excellent were 1.29 (95%CI 1.15, 1.45) times more likely to be frequent users of public transport and 1.53 (95%CI 1.33, 1.76) times more likely to choose to walk or cycle journeys of less than two to three miles. Frequent use of public transport was found to be consistently associated with better mental health for GHQ caseness (OR 0.85, 95%CI 0.79, 0.91), GHQ score (coefficient -0.28, 95%CI -0.41, -0.16), MCS (coefficient 0.45, 95%CI 0.23, 0.66), and WEMWBS (coefficient 0.30, 95%CI 0.19, 0.40). Among frequent users of public transport, participants expressing poor PPTI were 1.46 (95%CI 1.11, 1.93) times more likely to report poorer mental health according to the GHQ caseness indicator, compared to frequent users that regarded PPTI as excellent. Similar results were observed for the other indicators of mental health. Conclusions These findings indicate that while the provision of public transport infrastructure is a necessary pre-condition for stimulating population increases in physical activity, PPTI improvements needs to be prioritised to leverage the full mental health-related co-benefits of active travel.