Tungsten disulfide (WS2), as a representative layered transition metal dichalcogenide (TMDC) material, possesses important potential for applications in highly sensitive sensors. Here, a sensitivity-enhanced surface plasmon resonance (SPR) sensor with a metal film modified by an overlayer of WS2 nanosheets is proposed and demonstrated. The SPR sensitivity is related to the thickness of the WS2 overlayer, which can be tailored by coating a WS2 ethanol suspension with different concentrations or by the number of times of repeated post-coating. Benefitting from its large surface area, high refractive index, and unique optoelectronic properties, the WS2 nanosheet overlayer coated on the gold film significantly improves the sensing sensitivity. The highest sensitivity (up to 2459.3 nm/RIU) in the experiment is achieved by coating the WS2 suspension once. Compared to the case without a WS2 overlayer, this result shows a sensitivity enhancement of 26.6%. The influence of the WS2 nanosheet overlayer on the sensing performance improvement is analyzed and discussed. Moreover, the proposed WS2 SPR sensor has a linear correlation coefficient of 99.76% in refractive index range of 1.333 to 1.360. Besides sensitivity enhancement, the WS2 nanosheet overlayer is able to show additional advantages, such as protection of metal film from oxidation, tunability of the resonance wavelength region, biocompatibility, capability of vapor, and gas sensing.