A sustainable strategy based on chitin from waste seafood is proposed to remove nano‐size microplastics in water. A chitin nanofibrous foam is constructed by a new hydrogen bond rearrangement scheme without any crosslinking, which delivers an impressive high adsorption capacity of 411.14 ± 1.50 mg g−1 for small‐sized (< 1 µm) microplastics. This excellent adsorption capacity stems from the rough fibrous surface structure of the highly porous foam, the positively charged nature of the partially deacetylated chitin and other molecular interactions introduced by the activation and increased exposure of ‐OH, ‐NH2 and ‐NHCO‐ groups. Molecular dynamics simulation further demonstrates that C‐H‐π, O‐H‐π, and C = O‐π interactions between the microplastics and chitin foam facilitates the efficient removal of microplastics. A high removal efficiency is maintained even in salty water, a property that exemplifies good adaptability to various water bodies. Finally, two proof‐of‐principle scenarios are presented for converting the recovered microplastics into value‐added products. Thus, the entire cycling strategy represents a powerful remedy for the urgent yet challenging ocean microplastic pollution problem.