Abstract: To improve the capacity of adhesion and migration in vascular smooth muscle cells (vSMCs), the fiber surface was modified by having the electrospun aligned poly(lactic-lactide) (PLLA) ultrafine fibers individually coated with hyaluronic acid (HA) biomacromolecules via stable jet coaxial electrospinning (SJCES). First of all, under the condition of serum-free starvation, the effect of HA presence in the culture medium on promoting vSMC migration was examined. Then, highly-aligned HA-coated PLLA composite fibers (HA-PLLA) in shell-core structure were produced by SJCES, and the morphology, shell-core structure and mechanical properties of the HA-PLLA fibers were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), infrared spectroscopy (FT-IR), X-ray diffraction (XRD), and a universal mechanical tester. Finally, the efficacy of HA-PLLA fiber arrays in supporting vSMC migration was detected based on an improved "wound" healing method. Results showed that the presence of HA was capable of promoting vSMC migration. HA-PLLA aligned fibers in shell-core structure were successfully fabricated using SJCES. Modification of HA significantly improved the cytocompatibility of the aligned PLLA fibers, and enhanced their efficiency in directing vSMC migration, thus confirming the effectiveness of HA modification in promoting the migration of vSMCs on the aligned fibrous substrate of PLLA.