This study addressed a methodological gap by comparing psychological and social outcomes of exercise in green outdoors versus built indoors settings, whilst rigorously controlling exercise mode and intensity. The hypotheses were that greater improvements or more desirable values for directed attention, mood, perceived exertion, social interaction time, intention for future exercise behaviour and enjoyment would be associated with outdoors compared to indoors exercise. Following a baseline session, paired participants completed two conditions of 15 min of cycling on an ergometer placed outside in a natural environment and inside in a laboratory setting in a randomized, counter-balanced order. At pre- and post-exercise, directed attention was measured with the digit span backwards task, and mood was assessed with the Profile of Mood States. During the exercise session, visual and verbal interactions were recorded by means of experimenter observations. After each exercise session, participants provided self-reports of their enjoyment of the exercise, perceived exertion and intention for future exercise in the same environment. Social interaction time was significantly greater during outdoors exercise versus indoors; on average, participants engaged in three minutes more social interaction during exercise outdoors compared to indoors. Social interaction time significantly predicted intention for future exercise in the outdoors condition, but did not in the indoor condition. There was a significant time by condition interaction for directed attention. Scores worsened in the indoors condition, but improved in the outdoors condition. There was no statistically-significant time by condition interaction for mood and no significant difference between conditions for either perceived exertion or intention. Taken together, these findings show that exercise in a natural environment may promote directed attention and social interactions, which may positively influence future exercise intentions.