Silk fibroin (SF) is a biodegradable protein and possesses superior skin‐friendliness, biocompatibility, low immunogenicity, and non‐toxicity. However, SF has a series of drawbacks. For example, the application of SF in water filtration is limited by its inadequate ability to adsorb heavy metal ions. It is not inherently antibacterial, making SF ineffective as a filter to eliminate airborne bacteria. SF without conductivity is not suitable for use in sensors and triboelectric nanogenerators. In tissue engineering, deficient mechanical and anti‐inflammatory properties also have an influence on the rate of wound recovery. While physical and chemical modifications will improve its application properties as well as broaden its application areas. This review describes the modification of SF by filling, blending, structural adjustment, post treatment, crosslinking, grafting, and in situ polymerization to provide it with other functional properties. Modified SF fibers prepared by various methods (e.g., wet/dry/microfluidic spinning, electrospinning) are discussed, and they can be used in water/air filtration, chemical/pressure/strain sensors, triboelectric nanogenerators, artificial skin, wound dressings, and tissue scaffolds. Finally, the development trend of the modified SF fibers is prospected. This review has a reference significance on how to use modified SF fibers to improve filtration efficiency, sensor performance, and wound recovery.