Plasmonic nanostructures have been regarded as potential candidates for boosting the nonlinear up-conversion rate at the nanoscale level due to their strong near-field enhancement and inherent high design freedom. Here, we design a hybrid metasurface to realize the moderate interaction of Fano resonance and create the dual-resonant mode-matching condition to facilitate the nonlinear process of second harmonic generation (SHG). The hybrid metasurface presents dipolar and octupolar plasmonic modes near the fundamental and doubled-frequency wavelengths, respectively, further utilized to enhance the SHG of low-dimensional MoS2 semiconductors. The maximum intensity of SHG in hybrid metasurface coupled MoS2 is more than ten thousand times larger than that of other structure-units coupled MoS2. The conversion efficiency is reported to be as high as 3.27 × 10−7. This work paves the way to optimize nonlinear light–matter interactions in low-dimensional structures coupled with semiconductors.