Two-dimensional layered materials have attracted tremendous attention as photodetectors due to their fascinating features, including comprehensive coverage of band gaps, high potential in new-generation electronic devices, mechanical flexibility, and sensitive light-mass interaction. Currently, graphene and transition-metal dichalcogenides (TMDCs) are the most attractive active materials for constructing photodetectors. A growing number of emerging TMDCs applied in photodetectors bring up opportunities in the direct band gap independence with thickness. This study demonstrated for the first time a photodetector based on a few-layer ReMoS, which was grown by chemical vapor deposition (CVD) under atmospheric pressure. The detailed material characterizations were performed using Raman spectroscopy, photoluminescence, and X-ray photoelectron spectroscopy (XPS) on an as-grown few-layer ReMoS. The results show that both MoSand ReSpeaks appear in the ReMoSRaman diagram. ReMoSis observed to emit light at a wavelength of 716.8 nm. The electronic band structure of the few layers of ReMoScalculated using the first-principles theory suggests that the band gap of ReMoSis larger than that of ReSand smaller than that of MoS, which is consistent with the photoluminescence results. The thermal stability of the few layers of ReMoSwas evaluated using Raman temperature measurements. It is found that the thermal stability of ReMoSis close to those of pure ReSand MoS. The fabricated ReMoSphotodetector shows a high response rate of 7.46 A Wunder 365 nm illumination, offering a competitive performance to the devices based on TMDCs and graphenes. This study unambiguously distinguishes ReMoSas a future candidate in electronics and optoelectronics.