Poor mechanical properties and low photothermal efficiency of silk fibroin (SF)-based aerogels are current challenges that need to be addressed. Herein, SF composite aerogel was developed to enhance the mechanical properties through physical interpenetration of natural down fiber (Df) and hydrogen bonds formed among SF, Df, and polypyrrole (PPy) and to improve the evaporation performance via in-situ polymerization of PPy. The resultant Df/PPy@SF aerogel showed significant improvement of compressive stress (194.29 kPa), which was 6.96 times than that of SF aerogel (27.91 kPa), and also good compression resiliency. Furthermore, due to uniform distribution of PPy and high porosity of 95.27 %, Df/PPy@SF aerogel possessed high light absorbance of 99.87 % and low thermal conductivity (0.043 W·m−1·K−1). Thus, the Df/PPy@SF aerogel evaporator demonstrated high evaporation rates of 2.12 kg·m−2·h−1 for 3.5 wt% saline water, 2.04–2.15 kg·m−2·h−1 for various dye water, and 2.10 kg·m−2·h−1 for actual dye wastewater. Moreover, the developed aerogel exhibited evaporation stability and outstanding salt-resistance when treating seawater due to continuous water supply by superhydrophilic porous aerogel. Therefore, these findings demonstrate the excellent performance of Df/PPy@SF aerogel and will inspire further research on developing natural fiber-reinforced aerogels for use in the fields of solar water evaporation, energy, and other related applications.
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