Surface plasmon resonance (SPR) biosensors, with germanium sulfide (GeS) as a sensitive medium and Al/Ag/Au as the metal layers, are reported as we aim to improve the sensitivities of the biosensors. The sensitivities in conventional SPR biosensors, consisting of only metal Al, Ag, and Au layers, are 111°/RIU, 117°/RIU, 139°/RIU, respectively. Additionally, these sensitivities of the SPR biosensors based on the GeS-Al, GeS-Ag, and GeS-Au layers have an obvious improvement, resultant of 320°/RIU, 295°/RIU, and 260°/RIU, respectively. We also discuss the changing sensing medium GeS thickness using layer number to describe the scenario which brought about the diversification on the figure of merit (FOM) and optical absorption (OA) performance of the biosensors. These biosensors show obvious improvement of sensitivity and have strong SPR excitation to analytes; we believe that these kind biosensors could find potential applications in biological detection, chemical examination, and medical diagnosis.