This study investigated whether residential availability of natural outdoor environments (NOE) was associated with contact with NOE, overall physical activity and physical activity in NOE, in four different European cities using objective measures. A nested cross-sectional study was conducted in Barcelona (Spain); Stoke-on-Trent (United Kingdom); Doetinchem (The Netherlands); and Kaunas (Lithuania). Smartphones were used to collect information on the location and physical activity (overall and NOE) of around 100 residents of each city over seven days. We used Geographic Information Systems (GIS) to determine residential NOE availability (presence/absence of NOE within 300 m buffer from residence), contact with NOE (time spent in NOE), overall PA (total physical activity), NOE PA (total physical activity in NOE). Potential effect modifiers were investigated. Participants spent around 40 min in NOE and 80 min doing overall PA daily, of which 11% was in NOE. Having residential NOE availability was consistently linked with higher NOE contact during weekdays, but not to overall PA. Having residential NOE availability was related to NOE PA, especially for our Barcelona participants, people that lived in a city with low NOE availability.