Abstract: With the intensification of energy, materials, health, and resource issues, there is a growing need to develop new materials that combine functional usability, biosafety, and renewability. Silk fibroin, derived from natural silk, has processability, excellent mechanical properties, good biocompatibility, and controllable degradation characteristics. It shows great potential for applications in fields such as biomedicine, smart wearables, and flexible sensing. This article summarizes recent advances in the functionalization and intelligentization of silk fibroin-based materials. Building on our group's research findings, it highlights the research progress in silk fibroin-based fiber, film, 3D materials, biomedical scaffolds, self-powered devices and memristors. The review aims to provide guidance for the high-performance, multifunctional, and intelligent design and preparation of silk fibroin-based materials.