The surface morphology, thermal and mechanical properties of Bombyx mori silk fibroin (SF) fiber treated with a 1.23 N iodine-potassium iodide (I-2-KI) aqueous solution were investigated using scanning electron microscopy (SEM), atomic force microscopy (AFM), differential scanning calorimetry, thermogravimetric analysis, and tensile measurements to clarify the effects of the iodine treatment. SEM and AFM analyses indicated that the SF fiber surface became rougher by the absorption of polyiodide ions. The mechanical properties of iodinated SF showed an increase in Young's modulus, and strain remained constant although ultimate tensile strength slightly decreased. The thermal stability of SF molecules was greatly enhanced by iodine treatment. Iodinated SF fibers should be an attractive candidate for biomedical applications such as for producing antimicrobial filters, iodine containing wound-healing anion exchange fibers, etc.