Loneliness and social isolation are a growing public health concern, yet there are few evidence-based interventions for mitigating these social risk factors. Accumulating evidence suggests that mindfulness interventions can improve social-relationship processes. However, the active ingredients of mindfulness training underlying these improvements are unclear. Developing mindfulness-specific skills—namely, (i) monitoring present-moment experiences with (ii) an orientation of acceptance—may change the way people perceive and relate toward others. We predicted that developing openness and acceptance toward present experiences is critical for reducing loneliness and increasing social contact and that removing acceptance-skills training from a mindfulness intervention would eliminate these benefits. In this dismantling trial, 153 community adults were randomly assigned to a 14-lesson smartphone-based intervention: (i) training in both monitoring and acceptance (Monitor+Accept), (ii) training in monitoring only (Monitor Only), or (iii) active control training. For 3 d before and after the intervention, ambulatory assessments were used to measure loneliness and social contact in daily life. Consistent with predictions, Monitor+Accept training reduced daily-life loneliness by 22% (d = 0.44, P = 0.0001) and increased social contact by two more interactions each day (d = 0.47, P = 0.001) and one more person each day (d = 0.39, P = 0.004), compared with both Monitor Only and control trainings. These findings describe a behavioral therapeutic target for improving social-relationship functioning; by fostering equanimity with feelings of loneliness and social disconnect, acceptance-skills training may allow loneliness to dissipate and encourage greater engagement with others in daily life.