Aesthetic experiences, emerging saliently in the arts, play a pivotal role in transformative learning and creative processes that elicit physiological, affective, and cognitive responses associated with mental health indices. Interactions between subjects and aesthetic objects (e.g., visual artwork, music, and moving bodies) often entail elements of surprise and uncertainty that drive the inference of the hidden causes in the subject’s internal and external environment. These generate dynamics that align with the action-oriented Predictive Processing framework of brain function. Creative Arts Therapies (CATs) harness these dynamics by cultivating relational engagement using the arts modalities, prompting affective and cognitive processing. In this manuscript, we offer a review and conceptual analysis of recent empirical findings and theoretical premises that underpin aesthetic experiences and their relation to the psychotherapeutic use of the arts with a broad spectrum of populations and mental health conditions. We present a neuroscience-based approach to aesthetic intra- and inter-personal experiences, integrating therapeutic change factors of externalization-concretization, embodiment, and symbolization with functional network configurations, and interpersonal brain-to-brain coupling, to support predictive processing, learning, and creativity. Present and future interdisciplinary collaborations are underlined to elucidate the neurodynamic mechanisms driving psychological transformations, bridging neuroaesthetics and CATs.