Psychedelic substances have a long history of use in traditional healing and religious ceremonies worldwide and are increasingly being investigated for their possible therapeutic usage. However, there is still a lack of consensus regarding how best to characterize the psychological effects of psychedelics and how they bring about the positive therapeutic outcomes observed in clinical studies. The aim of this article is to review available evidence from quantitative and qualitative studies on psychedelic-assisted therapy, as well as neurobiological studies, in relation to the hypothesis that psychedelics facilitate the emergence of emotionally charged unconscious material, originally proposed by pioneering psychedelics researcher Stanislav Grof. The reviewed process studies of therapeutic mechanisms in psychedelic-assisted therapy and qualitative studies of treatment participants clearly indicate that the psychedelic experience is associated with the subjective experience of having increased access to and awareness of emotions, memories, and perceptions that are normally avoided or outside of conscious awareness. Brain-imaging studies point to several different neurobiological effects of psychedelics that might be related to these subjective psychological experiences. Available evidence also indicates that this process might constitute an important therapeutic mechanism in psychedelic-assisted therapy, worthy of further investigation.