Complex peripheral nerve injuries or defects, especially at branching sites, remain a prominent clinical challenge after the application of different treatment strategies. The current neural grafts cannot match the expected shape and size according to specific situations, cannot perform fine and precise branch nerve repair, and lack geometric and microscale regenerative navigation. In this study, we developed a personalized multi-level outer membrane/peripheral membrane/neural inner membrane simulation device (SpinMed) inspired by sugar painting to customize natural cues with selective protective sheaths and guiding cores to support rapid vascular reconstruction and effective neural process extension along the defect area. The biomimetic nerve bundle membrane determines the host guest cross-linking, in which the newly secreted vascular polymer 1 binds to the surface of silk fibroin filling as an anchor, helping to promote the homing of Schwann cells and the regeneration of myelin sheaths in the biological nerve inner membrane. After implantation of SpinMed into the sciatic nerve defect of rats, satisfactory results were achieved in structural reconstruction, with both sensory and motor functions restored. We further customized SpinMed grafts based on anatomy and digital imaging, achieving rapid repair of nerve trunks and branches in specific beagle neural defect models, which is superior to autologous and decellularized transplantation, and has reliable biocompatibility. Overall, this intelligent artistic biomimetic design provides a method for customizing complex high-performance neural grafts, which has enormous potential for application in translational regenerative medicine.