The development of functionalized braided wires coated with chitosan that can be used for tissue suturing and tissue regeneration is the subject of this work. Poly(l-lactic acid) (PLLA) braided wires were successfully fabricated by combining an electrospinning technique and alignment collection with a mini-type braiding method. The resulting PLLA wires with and without chitosan coating were characterized through a variety of methods including scanning electron microscopy (SEM), X-ray photoelectronic spectra (XPS) and tensile mechanical testing. Hemolytic property, kinetic hemostasis behavior, platelet adhesion, erythrocyte adhesion, and water uptake ability of the wires were explored. The results showed that a nearly comparable mechanical behavior of the braided wires with some commercial suture could be obtained with well-aligned fibers, and no significant difference in tensile performances were recognized with and without the introduction of chitosan. The PLLA wires coated with chitosan were found to have better prohemostatic activity than those without a chitosan coating.