This work presents the results of the reinforcement effects of regenerated silk fibroin solutions (SF) of Bombyx-Mori, Antheraea-Yamamai and Tussah on aged historic silk. Furthermore, Carboxymethyl-chitosan (CMC) was utilized as reinforcement and antibacterial filler to further improving the mechanical properties and antibacterial effects. To clarify the rationale behind this process, comprehensive characterization was applied, and a speculative explanation was provided. The results showed that Bombyx-mori and Tussah have better restoring effects than Antheraea-yamamai. CMC has good compatibility to the SF, and the addition of CMC has significantly contributed to the improvement the mechanical properties and thermal stability of the restored silk, which is due to the formation of chemical bonding, strong hydrogen bonding and the construction of polymer network structure. The enhancement of crystallinity and reduction of beta-turns structure indicate that the micro-defects in the crystallization zone of the aged silk has been restored, and the ordered arrangement in the long-range ordered structure has been improved within a certain range. It was found that the CMC acted as antifungal agents when introduced on the aged historic silk, reducing the growth of Aspergillus niger, Aspergillus flavus and Paecilomyces variotii to a certain extent, which were commonly found in storage areas of libraries. (C) 2018 Elsevier B.V. All rights reserved.