A straightforward, fast, and versatile technique is developed to fabricate nanofibrous scaffold with excellent hydrophilicity, mechanical properties, and biocompatibility for tissue engineering. The thermoplastic polyurethane (TPU) nanofiber is fabricated by utilizing electrospinning, and then its surface is modified through simply immersing it into cellulose nanofibrils (CNF) dispersion and subjecting to ultrasonication. The results show that the CNF particles are successfully absorbed on the surface of TPU nanofiber. By introducing CNF particles on the surface of TPU nanofiber, the hydrophilicity, mechanical properties of fabricated CNF‐absorbed TPU scaffold are significantly increased. Additionally, the adhesion and proliferation of human umbilical vein endothelial cells cultured on CNF‐absorbed TPU scaffold are prominently enhanced in comparison with those of cultured on TPU scaffold. These findings suggest that the ultrasound‐assisted technique opens up a new way to simply and effectively modify the surface of various scaffolds and the modified scaffold could be shown a great potential in tissue engineering.