Polyurethane-based scaffolds have been considered as a promising strategy for tissue regeneration. Herein, the polyurethane and carbon nanotubes electrospun scaffolds were modified by polyvinyl alcohol-3-glycidoxypropyl-trimethoxysilane after oxygen plasma treatment to improve physicochemical and in vitro properties for efficient bone reconstruction. Finally, the morphology of scaffolds, chemical characterization, surface roughness, bioactivity, hydrophilicity, cell attachment, cell viability, and alkaline phosphatase activity were investigated. According to microscopy results, bead free and smooth fibers were obtained using electrospinning while the degree of uniformity was reduced after the surface modification process. However, the modification process induced higher hydrophilicity and bioactivity to prepared scaffolds. In addition, the attachment and viability of the cells were improved as a function of surface modification. The expression of alkaline phosphatase especially in modified fibers confirmed the initial potential of scaffolds for bone tissue engineering applications and further studies.