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Pathological gambling (PG), a disorder currently categorized as an impulse-control disorder but being considered as a nonsubstance addiction in Diagnostic and Statistical Manual of Mental Disorders (5th ed.) discussions, represents a significant public health concern. Over the past decade, considerable advances have been made with respect to understanding the biological underpinnings of PG. Research has also demonstrated the efficacies of multiple treatments, particularly behavioral therapies, for treating PG. Despite these advances, relatively little is known regarding how biological measures, particularly those assessing brain function, relate to treatments for PG. In this article, we present a conceptual review focusing on the neurobiology of behavioral therapies for PG. To illustrate issues related to study design, we present proof-of-concept preliminary data that link Stroop-related brain activations prior to treatment onset to treatment outcome in individuals with PG receiving a cognitive–behavioral treatment incorporating aspects of imaginal desensitization and motivational interviewing. We conclude with recommendations about current and future directions regarding how to incorporate and translate biological findings into improved therapies for individuals with nonsubstance and substance addictions.