A grating-coupled terahertz (THz) surface plasmon polariton (SPP) resonant biochemical sensing structure is designed with simulation, which can be easily prepared by etching a submillimeter grating on the surface of indium antimonide (InSb) substrate. The simulation results based on the phase matching equation show that when the TM-polarized broadband terahertz collimated beam is incident on the InSb grating at a 30° angle, the low-frequency SPP and high-frequency SPP with opposite propagation directions can be simultaneously excited by the –1st and +1st order diffraction beams of the grating, respectively. Since the low-frequency SPP is easy to accurately measure with a commercial THz time-domain spectroscopy devices, the dependence of the resonance characteristics and sensing characteristics of low-frequency SPP on the grating structure parameters is systematically simulated in this paper. The simulation results show that the refractive-index sensitivity of the InSb grating-coupled THz-SPP resonant sensor chip decreases with the increase of the grating period, and is 1.05 THz/RIU at a grating period of 120 μm and an incident angle of 30°. Under these conditions, the sensor chip cannot make a detectable response to the monolayer adsorption of biomolecules, because the evanescent field penetration depth of the low-frequency SPP is much greater than the biomolecular size, resulting in insufficient field-biomolecular interaction at the surface. In order to detect biomolecules, a sensitivity enhancement method based on porous thin films is proposed and analyzed with simulation. The porous films enable not only to enrich biomolecules, but also to extend the interaction between THz-SPP and biomolecules from the molecular size to the entire film thickness, thereby improving the sensitivity of the sensor to biomolecular adsorption. Taking tyrosine adsorption as an example, the simulation results show that when the InSb grating is covered with a porous polymethyl methacrylate (PMMA) film with a thickness of 120 μm and a porosity of 0.4, the sensor sensitivity to tyrosine adsorption is 0.39 THz/unit volume fraction.