Bio-based triboelectric nanogenerators (TENGs) are expected to power medical device and detect real-time human motion behavior due to eco-friendliness and biocompatibility. However, the output performance of the TENGs needs to be boosted. In this study, a biodegradable silk fibroin-based TENG with enhanced output performance regulated by interfacial and ionic polarization is proposed. The friction layers, regenerated silk fibroin (RSF) film and silk nanoribbon (SNR) film, are functionalized through the induction of histidine with imidazolyl and lithium chloride, respectively, thus increasing the dielectric constant and triboelectric properties of friction layers. The enhancement is attributed to the enlarged difference of electron-absorbing ability and electron-donating ability of the two friction layers. The total silk fibroin-based TENG shows a maximum voltage of 63.0 V, and a current of 2.4 μA. Moreover, the obtained maximum power density of 828.8 mW m