Non-carbonized photothermal conversion materials (PTCMs) created from polysaccharides are highly intriguing but unexplored for the lacked light-absorbing groups. Meanwhile, macromolecular PTCMs operate as single molecules enable optimal solar
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thermal conversion remains challenge. Herein, we employ a molecular engineering strategy to enhance chitosan's absorption by incorporating robust-light-absorbing carbonyl groups to fabricate oxidized chitosan (OCTS) with 408 % enhancements in solar
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thermal conversion efficiency due to full-spectrum solar absorption. Then the water-soluble OCTS is utilized to fabricate gelatin/OCTS/K
3Cit/ethylene glycol (GOKE) polyelectrolyte organohydrogel with excellent solar
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thermal-induced self-healing, ultrastrong mechanical and antibacterial properties. The incorporation of OCTS facilitates GOKE to harvest over 98 % full-spectrum solar absorption, 92 % solar
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thermal driven self-healing efficiency after five cycles, and tensile strength and toughness of 5.53 MPa and 9.81 MJ m
3 attributed to Hofmeister effect strategy. Encouragingly, benefiting from OCTS's excellent solar
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thermal conversion and polyelectrolyte properties, GOKE is assembled into solar
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thermal
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electric generators (STEG) and triboelectric
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nanogenerators (TENG), showing dual-mode electric output (50.3 mA/16.4 W m
2 for STEG and 37 V/16.2 mW m
2 for TENG). Additionally, GOKE-based flexible supercapacitors exhibit energy density of 11.3 Wh kg
1 and specific capacitance of 81.5 F g
1, capable of storing energy generated by STEG/TENG. Noteworthy, this study pioneers polysaccharide-based non-carbonized PTCMs with potential applications in clean energy production/storage.