Commercially available GBR membranes include polytetrafluoroethylene (PTFE), poly (ε-caprolactone)(PCL), polylactic acid (PLA), polyglycolic acid (PGA), collagen, and so on. [4,5] The ideal GBR membrane should be biocompatible, degradable, and have favorable mechanical properties. [6] However, most commercial GBR membranes are either nondegradable, or not stiff enough to match bone, which limits their application in bone regeneration.Incorporation of functional nanoparticles in GBR membranes would be an effective strategy for elevation of their performance. Bioactive inorganic nanofillers, such as graphene oxide, [7] octacalcium phosphate, [8] and bioactive glass, [9] have been incorporated into GBR membranes to improve the stiffness or osteoconductivity. Recently, nanosized molybdenum disulfide (MoS 2 ) has attracted much attention in biomedical field owing to its fantastic physiochemical properties, biocompatibility, and excellent bioactivities. MoS 2 exhibits low cytotoxicity and genotoxicity, [10,11] since Mo is an important trace element for humans that acts as a cofactor for many redox enzymes and S is also an abundant biological element. [12,13] The addition of MoS 2 in polymers, such as polyacrylonitrile/MoS 2 , chitosan/MoS 2 , and poly vinylidene fluoride/MoS 2 , has been demonstrated to promote cell proliferation. [14][15][16] MoS 2 was also found to have an osteogenic potential. Zhang et al. documented that the nanostructured Electrospun nanofiber membranes have been widely used for guided bone regeneration (GBR). For assistance in bone healing, photothermal therapy which renders moderate heat stimulation to defect regions by near-infrared (NIR) light irradiation has attracted much attention in recent years. Combined with photothermal therapy, novel electrospun poly(ε-caprolactone)/ molybdenum disulfide (PCL/MoS 2 ) nanofiber membranes are innovatively synthesized as GBR for bone therapy, wherein the exfoliated MoS 2 nanosheets served as osteogenic enhancers and NIR photothermal agents. With the doping of MoS 2 , the mechanical properties of nanofiber membranes got improved with the degradation unaffected. The composite PCL/MoS 2 membranes show enhanced cell growth and osteogenic performance compared with PCL alone. Under NIR-triggered mild photothermal therapy, osteogenesis and bone healing are accelerated by using PCL/MoS 2 nanofiber membranes for growth of bone mesenchymal stem cells in vitro and repair of rat tibia bone defect in vivo. The novel nanofiber membranes may be developed as intelligent GBR in the therapy of bone defects.