According to psychological theories of environmental affect, the physical environment moderates the walking experience and its psychological wellbeing benefits. The present paper further demonstrates that affective experiences also influence intentions to walk. A study to explore the influence of affective experiences of walking on walking intentions is reported. A sample of adults working or studying in Bristol, UK (n = 384) participated in an experiment involving virtual exposure to one of five environments, with evaluations of their affective experience and of intentions to walk in the setting. A subsample (n = 14) then took part in photo-elicited semi-structured interviews. Multiple regression analyses showed that affective experiences of walking influenced walking intentions. Interview analyses highlighted the role of traffic, city busyness, and poor aesthetics. This is the first empirical study that examines the walking experience and related walking intentions from the pedestrian perspective employing theories of environmental affect. The findings indicate that safety, comfort, and moderate sensory stimulation are crucial elements for the walking experience. Following this, a strategy to promote active mobility in the built environment can be constructed around safety, comfort, and moderate sensory stimulation by targeting the micro elements that prevent them.