The silk-based bionanohybrids have been an innovative choice for the current researcher to utilize them for the removal of heavy metals from wastewater. These silk-based bionanohybrids are combination of natural protein fiber and silk fibroin which then combined with different nanomaterials that provides hope for the environmental remediation. Due to different advantages such as biodegradability and biocompatibility, the silk fibroin is being used advanced applications. Silk fibroin exhibits excellent metal binding characteristics due to its exceptional structural features and functional groups, e.g., carboxyls and amines which can form a coordination bond with the metal ions. Moreover, incorporation of nanomaterials into the silk fibroin such as carbon nanorods and nanotubes that increases the metal removal efficiency proposed material. In addition, the silk-based bionanohybrids exhibits exceptional properties of metal removal making it promising material for environmental remediation. This chapter will focus on the fabrication of various silk-based bionanohybrids and their applications as an adsorbent for the removal heavy metal ions.