Surface-enhanced Raman scattering (SERS) substrates based on chemical mechanism (CM) have received widespread attentions for the stable and repeatable signal output due to their excellent chemical stability, uniform molecular adsorption and controllable molecular orientation. However, it remains huge challenges to achieve the optimal SERS signal for diverse molecules with different band structures on the same substrate. Herein, we demonstrate a graphene oxide (GO) energy band regulation strategy through ferroelectric polarization to facilitate the charge transfer process for improving SERS activity. The Fermi level (E_f) of GO can be flexibly manipulated by adjusting the ferroelectric polarization direction or the temperature of the ferroelectric substrate. Experimentally, kelvin probe force microscopy (KPFM) is employed to quantitatively analyze the E_f of GO. Theoretically, the density functional theory calculations are also performed to verify the proposed modulation mechanism. Consequently, the SERS response of probe molecules with different band structures (R6G, CV, MB, PNTP) can be improved through polarization direction or temperature changes without the necessity to redesign the SERS substrate. This work provides a novel insight into the SERS substrate design based on CM and is expected to be applied to other two-dimensional materials.