Traditional medicinal plants in various countries, particularly in India have been used for centuries for various ailments; however, there has been little scientific effort to validate these anecdotal uses mentioned in the literature. A number of these traditionally used plant extracts and various "Ayurvedic medicines" that are highly valued in Ayurveda, the traditional system of medicine in India for antiaging, memory-enhancing, nerve tonic, anxiolytic, anti-inflammatory and immunopotentiation, have been screened using National Institutes of Mental Health (NIMH) Synthetic Screening Program for scientific validation and the development of new leads of psychotherapeutic compounds using Radioligand Receptor Binding Assays (RRA). Crude methanolic extracts of plants are screened using approximately 40 different in vitro RRA (primarily from rat brain homogenates) and 6 enzyme assays including acetylcholine esterase, choline acetyltransferase, and monoamine oxidase (MAO), A and B. The total crude extracts of many of these plants showed potent selectivity to various receptors, especially gamma-Amino Butyric Acid (GABA(A)), N-Methyl-D-Aspartic Acid (NMDA), and MAO receptors, which are presumed to be involved in mental disorders. The focus was on plants showing the highest displacement of GABA, cholecystokinin (CCK), NMDA, MAO, and benzodiazopines. Bioassay guided fractionation of the most active extracts resulted in pure compounds which retained the original activity of the crude extract validating the folkloric use. A bioactivity-guided fractionation of Terminalia bellerica fruit extract led to the isolation of several pure compounds which retained the original activity of the crude extract for CCK and GABA receptors, with the exception of compound B3EA-6, which exhibited high affinity for Neurokinin receptor (Substance K approximately NK-1). The absolute structure of B3EA-6 has been established by x-ray crystallography.