Links between wellbeing and environmental factors are of growing interest in psychology, health, conservation, economics, and more widely. There is limited evidence that green or natural environments are positive for physical and mental health and wellbeing. We present a new and unique primary research study exploring the relationship between momentary subjective wellbeing (SWB) and individuals' immediate environment within the UK. We developed and applied an innovative data collection tool: a smartphone app that signals participants at random moments, presenting a brief questionnaire while using satellite positioning (GPS) to determine geographical coordinates. We used this to collect over one million responses from more than 20,000 participants. Associating GPS response locations with objective spatial data, we estimate a model relating land cover to SWB using only the within-individual variation, while controlling for weather, daylight, activity, companionship, location type, time, day, and any response trend. On average, study participants are significantly and substantially happier outdoors in all green or natural habitat types than they are in urban environments. These findings are robust to a number of alternative models and model specifications. This study provides a new line of evidence on links between nature and wellbeing, strengthening existing evidence of a positive relationship between SWB and exposure to green or natural environments in daily life. Our results have informed the UK National Ecosystem Assessment (NEA), and the novel geo-located experience sampling methodology we describe has great potential to provide new insights in a range of areas of interest to policymakers.