Metasurfaces able to concentrate light at various wavelengths are promising for enhancing nonlinear interactions. In this Letter, we experimentally demonstrate infrared second-harmonic generation (SHG) by a multi-resonant nanostructure. A 100 GaAs layer embedded in a metal-insulator-metal waveguide is shown to support various localized resonances. One resonance enhances the nonlinear polarization due to the transverse magnetic (TM)-polarized pump wavelength near 3.2µm, while another is set near the TE-polarized generated wavelength (1.6µm). The measured SHG efficiency is higher than 10-9W-1 for pump wavelengths ranging from 2.9 to 3.3µm, which agrees with theoretical computations. This is typically 4 orders of magnitude higher than the equivalent GaAs membrane.