We report large emissivity and extraordinarily narrowband thermal radiation output from polyimide molecular vibrational modes, coupled to localized plasmon resonances supported by metal-insulator-metal (MIM) metasurfaces. The efficient coupling is facilitated by the strong localization of resonant radiation field in the thin-film polyimide insulator layer, as illustrated in Fig. . Coupling strength dependent interactions between MIM resonant modes and the modal structure of polyimide vibrational spectrum were modeled theoretically and systematically studied experimentally by varying top layer metal disk diameters . Furthermore, metasurfaces were fabricated using highly scaleable and cost effective optical lithography methods, and the polyimide absorber film was selected for its compatibility with both semiconductor CMOS process and thermal treatments up to ∼ 300 • C. The investigated structures exhibit a remarkable agreement between theoretical and experimental findings, and provide a way to devise highly tailored planar MIR radiation sources which for their spectral signatures can draw upon a rich variety of molecular compounds.