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This chapter examines the scientific and clinical foundations of traditional herbal anxiolytics within the emerging field of neurophytomedicine. It explores the global prevalence and neurobiology of anxiety disorders, limitations of conventional pharmacological treatments, and the therapeutic potential of botanicals with historical use in anxiety relief. Emphasis is placed on phytochemical classes such as flavonoids, terpenes, alkaloids, and saponins, and their mechanisms of action on GABAergic, serotonergic, and hypothalamic pituitary adrenal systems. Comparative clinical evidence, safety considerations, herb-drug interactions, and regulatory frameworks are critically reviewed. The chapter also addresses challenges in standardization, placebo effects in trials, and ethical sourcing of medicinal plants. Finally, it outlines future directions including pharmacogenomic personalization, AI-driven phytochemical discovery, and integration of validated botanicals into mainstream psychiatry.