Regenerated keratin-based adsorbents have attracted much attention in environmental pollution remediation. However, fabricating keratin-based adsorbents with excellent adsorption performance is still a challenging issue due to its weak mechanical property. In this study, mechanical robust keratin composite films were designed and engineered at mesoscopic scale by molecular network reconstruction strategy. It was found that the beta-crystallites structure of silk fibroin template could induce the transformation of free unfolded molecular chains of keratin to beta-sheet conformation and further resulted in the controllable manipulating of the mechanical properties of keratin films. This mechanical reinforced composite film showed high adsorption efficiency and capacity for dyes as well as ideal regeneration and recycling performance. Adsorption behavior of reactive brilliant blue KN-R by keratin composite films was comprehensively studied. The adsorption capacity (q(e)) and removal efficiency for KN-R by the adsorbent could reach as high as 190.84 mg/g and 98.52%, respectively. The adsorbent exhibited excellent regeneration and recycling performance due to its mechanical robustness. The molecular network reconstruction strategy is both straightforward and effective for fabricating mechanical robust adsorbent for pollutant remediation. (C) 2020 Elsevier Inc. All rights reserved.