Aerogels are becoming a promising platform to fabricate photothermal materials for use in solar steam generation (SSG), which have remarkable application potential in solar desalination, due to their excellent thermal management, salt resistance, and considerable water evaporation rate. In this work, a novel photothermal material is fabricated by forming a suspension between sugarcane bagasse fibers (SBF) and poly(vinyl alcohol), tannic acid (TA), and Fe 3+ solutions via hydrogen bonds of hydroxyl groups. After freeze drying, the fabricated SBF aerogel-based photothermal (SBFAP) material possesses a 3D interconnected porous microstructure, which could enhance water transportation ability, reduce thermal conductivity, and quickly dissolve salt crystals on the SBFAP surface. Thanks to the formation of micro/nanosized complexes between TA and Fe 3+ ions on the SBFAP material, the SBFAP exhibits high light capture and water evaporation rate (2.28 kg m −2 h −1 ). In particular, due to strong hydrogen bonding and the SBF, the SBFAP material is reinforced, thereby exhibiting excellent structural stability in seawater. Moreover, the high salt tolerance of SBFAP favors its high desalination performance for at least 76 days of continuous evaporation under actual conditions. This research paves the way for the fabrication of natural cellulose fiber-based photothermal materials for application in solar desalination.