The effects and action mechanism of tea polyphenols (TP) on the quality of rapeseed oil during frying process were investigated. Results showed that compared with control, TP (0.04%, w/w) exhibited the remarkable ability to inhibit the deterioration of acid value, peroxide value, anisidine value, viscosity, and color of frying oil. By using gas chromatography-mass spectrometry, frying oil with TP showed the higher content of unsaturated fatty acids (72.79%) and lower content of trans fatty acids (3.36%) than those of control. Meanwhile, frying oil with TP had a higher total phenolic content than control at the same frying time. In addition, the thermo gravimetric-differential scanning calorimetry results showed that TP could increase the oxidation stability of rapeseed oil. Furthermore, according to the Fourier transform infrared and molecular dynamic simulation results, TP could reduce the breaking degree of = C-H bond, C-O-C bond, and C = C bond in oil molecules, and inhibit the oxidation of oil components by inhibiting the generation of free radicals and eliminating free radicals. All present results suggested that TP showed the potential value to be used for protecting the quality of oil during the frying process in food and chemical industries. PRACTICAL APPLICATIONS: The inhibitory effect of tea polyphenols on the deterioration of quality of rapeseed oil during frying was found and the mechanism had also preliminarily interpretation. This work provided a method for monitoring the quality of fry oil and provided the theoretical basis for the use of tea polyphenols in frying.