To enhance physicomechanical properties and bioactivity of fibrous membranes for wound dressing and tissue engineering applications, novel composite scaffolds consisting of fibrous mats and thermosensitive hydrogel particles were prepared by concurrent electrospinning and electrospraying technique. The composite scaffolds were composed of keratin/bacterial cellulose fibers (150 ± 43 nm) which are hybridized with hydrogel particles (500 nm to 2 μm) based on nonionic triblock copolymers conjugated with Tragacanth gum (TG). FTIR and H-NMR studies indicated ester reactions between carboxylated copolymers and TG through carbodiimide crosslinker chemistry. The hydrogel particles were uniformly embedded into fibrous network at fiber junctions without changing its porous structure and the fiber diameter. Modification of the fibers with the hydrogel nanoparticles significantly improved the hydrophilicity (~23%), module of elasticity (~31%), tensile strength (~35%), and ductility (~23%) of the electrospun scaffold. In vitro culturing of the mats with L929 fibroblast cells determined the biocompatibility of the fibrous composite along with improved cell adhesion and proliferation.