Background Emotional awareness and self-regulation are important skills for improving mental health and reducing the risk of cardiovascular disease. Cognitive behavioral therapy can teach these skills but is not widely available. Objective This exploratory study examined the potential of mobile phone technologies to broaden access to cognitive behavioral therapy techniques and to provide in-the-moment support. Methods We developed a mobile phone application with touch screen scales for mood reporting and therapeutic exercises for cognitive reappraisal (ie, examination of maladaptive interpretations) and physical relaxation. The application was deployed in a one-month field study with eight individuals who had reported significant stress during an employee health assessment. Participants were prompted via their mobile phones to report their moods several times a day on a Mood Map—a translation of the circumplex model of emotion—and a series of single-dimension mood scales. Using the prototype, participants could also activate mobile therapies as needed. During weekly open-ended interviews, participants discussed their use of the device and responded to longitudinal views of their data. Analyses included a thematic review of interview narratives, assessment of mood changes over the course of the study and the diurnal cycle, and interrogation of this mobile data based on stressful incidents reported in interviews. Results Five case studies illustrate participants' use of the mobile phone application to increase self-awareness and to cope with stress. One example is a participant who had been coping with longstanding marital conflict. After reflecting on his mood data, particularly a drop in energy each evening, the participant began practicing relaxation therapies on the phone before entering his house, applying cognitive reappraisal techniques to cope with stressful family interactions, and talking more openly with his wife. His mean anger, anxiety and sadness ratings all were lower in the second half of the field study than in the first (P ≤ .01 for all three scales). Similar changes were observed among other participants as they used the application to negotiate bureaucratic frustrations, work tensions and personal relationships. Participants appeared to understand the mood scales developed for this experience sampling application and responded to them in a way that was generally consistent with self-reflection in weekly interviews. Interview accounts of mood changes, associated with diurnal cycles, personal improvement over the course of the study, and stressful episodes, could be seen in the experience sampling data. Discrepancies between interview and experience-sampling data highlighted the ways that individuals responded to the two forms of inquiry and how they calibrated mood ratings over the course of the study. Conclusions Participants quickly grasped the Mood Mapping and therapeutic concepts, and applied them creatively in order to help themselves and empathize with others. Applications developed for mobile phones hold promise for delivering state-of-the-art psychotherapies in a nonstigmatizing fashion to many people who otherwise would not have access to therapy.