To investigate the effects of processing with different types of tea infusions on the phenolic components in herbal medicines, this study utilized the Zhuang medicine Tylophora ovata as a model to evaluate the content variations of its characteristic constituents, p-hydroxyacetophenone and paeonol, and to elucidate the underlying mechanisms. High-performance liquid chromatography (HPLC) was employed for quantitative analysis. Ultraviolet (UV) spectroscopy combined with molecular docking was utilized to exclude detection interference from the physical complexation of alkaloids, specifically caffeine and tylophorine. Furthermore, a simulated processing system was established to evaluate the impact of tea polyphenols on the retention rates of these phenolic compounds. Quantitative results indicate that, compared with the raw sample group, the content of p-hydroxyacetophenone significantly increased in the green tea-, white tea-, and dark tea-processed groups, but significantly decreased in the black tea- and yellow tea-processed groups. Meanwhile, paeonol levels declined across all tea infusion-processed groups, with reduction rates ranging from 4.0% to 11.4%. Mechanistic studies confirm that the binding affinities between the two phenolic compounds and the primary alkaloids were exceedingly weak, ensuring their physicochemical independence. The universal depletion of paeonol was primarily governed by high-temperature physical volatilization, upon which tea polyphenols exerted limited influence. In contrast, the variation in p-hydroxyacetophenone content was dictated by a dynamic competition between “thermal dissolution-induced release”and “oxidative degradation-induced consumption”, wherein tea polyphenols provided substantial antioxidant protection. This study clarified the chemical mechanisms by which different tea infusions modulate the retention of phenolic compounds, providing a scientific basis for the rational selection of specific tea types as processing excipients for toxic ethnomedicines.