Photonic structures with optical resonances beyond a single controllable mode are strongly desired for enhancing light-matter interactions and bringing about advanced photonic devices. However, the realization of effective multimodal photonic structures has been restricted by the limited tunable range of mode manipulation, the spatial dispersions of electric fields or the polarization-dependent excitations. To overcome these limitations, we create a dualmode metasurface by integrating the plasmonic surface lattice resonance and the gap plasmonic modes; this metasurface offers a widely tunable spectral range, good overlap in the spatial distribution of electric fields, and polarization independence of excitation light. To show that such dual-mode metasurfaces are versatile platforms for enhancing light-matter interactions, we experimentally demonstrate a significant enhancement of second-harmonic generation using our design, with a conversion efficiency of 1–3 orders of magnitude larger than those previously obtained in plasmonic systems. These results may inspire new designs for functional multimodal photonic structures.