Aerogels with low density, high mechanical strength, and excellent elasticity have a wide potential for applications in wastewater treatment, thermal management, and sensors. However, the fabrication of such aerogels from biomass materials required complex preparation processes. Herein, a sustainable and facile strategy was reported to construct lignin/cellulose aerogels (LCMA) with three-dimensional interconnected structures by introducing homologous lignin with a polyphenyl propane structure as a structural enhancer through a top-down directional freezing approach, prompting a 2036% enhancement in compressive modulus and an 8–12-fold increase in oil absorption capacity. In addition, the hydrophobic aerogels with superelasticity were achieved by combining the aligned polygon-like structure and flexible silane chains, which exhibited remarkable compressional fatigue resistance and superhydrophobicity (WCA = 168°). Attributed to its unique pore design and surface morphology control, the prepared aerogel exhibited excellent performance in immiscible oil–water separation and water-in-oil emulsion separation. Due to the ultra-low density (8.3 mg·cm–3) as well as high porosity (98.87%), the obtained aerogel showed a low thermal conductivity (0.02565 ± 0.0024 W·m–1·K–1), demonstrating a potential in insulation applications. The synthetic strategy and sustainability concept presented in this work could provide guidance for the preparation of advanced biomass-based aerogels with unique properties for a wide range of applications.
