This study aimed to evaluate the effect of theaflavins [TFs] on the process of dentin erosion and investigation the potential mechanism. For erosion kinetics of the dentin, 7 experimental groups (n = 5) treated with 10% ethanol [EtOH] (negative control) are erosion for 1, 2, 3, 4, 5, 6, and 7 d erosion cycles (4 cycles/d). For the effect of TFs on dentin erosion, 6 experimental groups (n = 5) were treated with 1% epigallocatechin gallate [EGCG], 1% chlorhexidine [CHX], 1%, 2%, 4%, and 8% TFs for the 30 s and then subjected to erosion cycles (4 cycles/d for 7 d). The erosive dentin wear (μm) and surface morphology were evaluated and compared by laser scanning confocal microscope and scanning electron microscopy. The matrix metalloproteinase inhibition effects of TFs were investigated using in situ zymography and molecular docking. TFs-treated collagen was investigated by ultimate microtensile strength, Fourier-transform infrared spectroscopy, and molecular docking. Data were analyzed by ANOVA, Tukey’s test (P< 0.05). The TFs-treated groups (7.56 ± 0.39, 5.29 ± 0.61, 3.28 ± 0.33, and 2.62 ± 0.99 μm for 1%, 2%, 4%, and 8% TFs) had significantly lower erosive dentin wear than the negative control group (11.23 ± 0.82 μm), and the effect was concentration-dependent at low concentrations (P< 0.05). TFs inhibit matrix metalloproteinase [MMP]. Moreover, TFs crosslink dentin collagen and cause hydrophilic changes in dentin collagen. TFs preserve organic matrix within the demineralized dentin by inhibiting MMP activity and simultaneously improving collagen’s resistance to enzymes, both of which contribute to preventing or slowing down the progression of dentin erosion.