Suicide is the leading cause of death in young people around the world, with depression as a major driver of these numbers. However, a substantial percentage of young people with depression do not seek professional help. As people in this demographic report listening should be to up to 5 hrs of music per day, music has the potential to serve as an effective method of reaching young people and increase their mental health literacy. MoodyTunes is an in-development mHealth app that aims to increasing mental health awareness in young people and to inform young people about how music can be used as an effective tool for self-regulating mood. Here, we report a mixed methods usability study of MoodyTunes in which a sample of young people (N = 20, age range: 12–25) experienced the app for the first time. A think-aloud method was used to evaluate the app, alongside quantitative survey responses, automated facial analysis data, and interview data. Survey data indicated that the app was perceived in a positive manner, and as effective and well-functioning, whereas aesthetic appeal received the lowest score. As hypothesized, women and younger participants displayed more positive emotions while using the app. Qualitative data indicated several positive aspects such as links to mental health resources and the ability to share music with others, but also highlighted the need to improve the aesthetic appeal, ease of use, and capacity to personalize the app. Future considerations and approaches for mHealth apps, as well as limitations in the present study, are discussed.