There are concerns about mental wellbeing in later life in older people as the global population becomes older and more urbanised. Mobility in the built environment has a role to play in improving quality of life and wellbeing, as it facilitates independence and social interaction. Recent studies using neuroimaging methods in environmental psychology research have shown that different types of urban environments may be associated with distinctive patterns of brain activity, suggesting that we interact differently with varying environments. This paper reports on research that explores older people’s responses to urban places and their mobility in and around the built environment. The project aim was to understand how older people experience different urban environments using a mixed methods approach including electroencephalography (EEG), self-reported measures, and interview results. We found that older participants experience changing levels of “excitement”, “engagement” and “frustration” (as interpreted by proprietary EEG software) whilst walking between a busy built urban environment and an urban green space environment. These changes were further reflected in the qualitative themes that emerged from transcribed interviews undertaken one week post-walk. There has been no research to date that has directly assessed neural responses to an urban environment combined with qualitative interview analysis. A synergy of methods offers a deeper understanding of the changing moods of older people across time whilst walking in city settings.