In this chapter, we review the latest research on the neuroscience and therapeutic potential of ayahuasca. Currently, the type of research available ranges from in vitro experiments to clinical studies performed to assess the modulation of neural and psychological processes. We also discuss the most recently reported findings, including (a) the neurobiological effects of ayahuasca, (b) the psychological mechanisms underlying the potential therapeutic effects of ayahuasca, (c) ayahuasca-induced metabolic and connectivity changes, and (d) the possible link with mindfulness-related capacities and emotion regulation. We also examine the effects of ayahuasca at the cellular level to better explore the role of β-carbolines and the neurogenetic properties of these alkaloids. These important findings indicate that these compounds, which still play a minor role in the overall pharmacology of ayahuasca, merit greater attention. Our aim is to show the remarkable versatility of ayahuasca as a therapeutic agent. Ayahuasca interacts with the brain–mind complex on multiple levels, and could be a powerful tool to help patients with neuropsychiatric disorders who are unable to find relief through currently available treatments.