This study delves into the transformative effects of atmospheric cold plasma (CP) treatment on little millet flour (LMF), specifically exploring alterations in bioactive compounds, antinutritional factors, and functional properties. Foaming and emulsification properties experienced noteworthy enhancements with plasma treatment, manifesting in significant increases in foaming capacity (up to 51.47 ± 0.49%), foaming stability, emulsification ability, and emulsion stability (up to 47.02 ± 0.35%). The treatment also positively influenced water absorption index and swelling power. Antinutritional factors, including tannins and saponins, exhibited substantial reductions following plasma treatment. Saponin content, for instance, decreased by an impressive 58% after exposure to 20 kV for 20 min. Conversely, bioactive compounds such as phenolic content and antioxidant activity saw significant increases. Total phenolic content (TPC) rose from 527.54 ± 8.94 to 575.82 ± 3.58 mg GAE/100 g, accompanied by a remarkable 59% boost in antioxidant activity. Interestingly, plasma treatment did not exhibit a discernible effect on pasting properties. These findings collectively underscore the potential of atmospheric CP treatment as a novel and effective method for enhancing the functional and nutritional attributes of LMF, thereby opening new avenues for its application in food science and technology.