The Paliyar tribe of Kadamalaikundu, Theni District of Tamil Nadu, India, has been deeply associated with forestry and ethnomedicinal practices for ages. The study aimed to identify the important medicinal plant species used by this tribe for ethnomedicinal purposes in the local vicinity. Eighty-nine informants were interviewed using the ‘specimen display’ and forest walk method, semi-structured open-ended questionnaires, interviews, and personal observations. The people from the region reported ninety-three plant species having medicinal properties. The Solanaceae family was recorded as the most dominant plant family, reporting seven different species of medicinal plants, followed by six species of the Acanthaceae family. In the study, Coccinia grandis had the highest use value (2.5), followed by Withania somnifera (2). In contrast, Cardiospermum halicacabum, Gossypium hirsutum, and Ocimum tenuiflorum with use value (1) and the ICF (Informant Consensus Factor) of value 1 accounted for 15 diseases out of forty-one categorized ailments. This study confirmed that the Paliyar tribe was dependent on a large number of medicinal plants for their primary healthcare and veterinary well-being, which require immediate conservation owing to their population fragmentation and the reluctance of the younger generation to adopt ethnomedicinal practices as occupation, which could lead to the loss of traditional knowledge as well. The study also documented the various important medicinal plant uses that could pave the way to the new pharmacological dimensions for modern wellness programs.