Polaritons in two-dimensional van der Waals (vdW) materials possess extreme light confinement, which have emerged as a potential platform for next-generation biosensing and infrared spectroscopy. Here, we propose an ultra-thin and electric tunable graphene/hexagonal boron nitride/graphene metasurface for detecting molecular fingerprints over a broad spectrum. The vdW metasurface supports hybrid plasmon–phonon polariton resonance with high-quality factor (Q > 120) and electrically controlled broadband spectra tunability from 6.5 to 7 μm. After coating a thin layer of bio-molecular (e.g., CBP) on top of the metasurface, the molecular absorption signatures can be readout at multiple spectral points and, thus, achieve broadband fingerprint retrieval of bio-molecules. Additionally, our electric tunable metasurface works as an integrated graphene-based field-effect transistor device, without the need of multiple resonance generators such as angle-resolved or pixelated dielectric metasurfaces for broadband spectra scanning, thereby paving the way for highly sensitive, miniaturized, and electrically addressed biosensing and infrared spectroscopy.