The combination of the electrochemiluminescence (ECL) technique with nanophotonics research can spark new analytical and sensing applications. Herein, we developed a novel modulation strategy of the ECL polarization angle based on the dynamically tunable few-layer metasurface. The bilayer metasurface consisted of a fixed Au-Ag core-shell nanocube array (Au@Ag NCA) layer with strong plasmonic hot spots and different amounts of the Au nanoparticles@MoS2 heterostructure nanosheet (0D-2D HNS) layer with strong metal-support interaction. Due to the interference and near-field coupling between layers, the bilayer metasurface can strongly redistribute the local electromagnetic field and energy in the ECL system, which not only significantly amplified the ECL signal but also modulated the polarization coupling angle. Therefore, the novel ECL polarization angle-resolved sensing strategy has been developed, which was beneficial to improve the sensitivity and resolution of ECL sensing. A dynamically tunable metasurface-based ECL biosensor was successfully used to detect the asthma-related miRNA-142-3p (miR-142-3p). Moreover, the simulation calculations of the electromagnetic field revealed the unique optical activity of the metasurface. This study brought the insightful understanding of the metasurface-modulated optical signal and provided a new idea to construct novel sensing platforms.