Solar-driven interfacial evaporation co-generation (SIE-CG) technology is of great significance in solving the problem of water and energy shortage. Herein, we report the ionic liquid-assisted alignment of waste biomass tea residue-based microcrystalline cellulose for aerogels (abbreviated as TPPA-5) with aligned channels for solar-driven interfacial evaporation cogeneration. In the ionic liquid, strong H-bonding is formed between the pyranoid rings of cellulose combined with the slow freezing technique, resulting in the microcrystalline cellulose being reoriented, which allowed TPPA-5 to form abundant aligned channels after solvent replacement and freeze-drying. These aligned channels enable the brine to form a localized circulating flow, which is conducive to the improvement of the TPPA's evaporation rate and salt resistance. The salinity gradient is naturally formed in the channel of TPPA, which enables TPPA-5 to show excellent power generation performance. The evaporation rate of TPPA-5 can reach 3.39 kg m −2 h −1 under 1 kW m −2 . With methanol as a highly polar proton solvent, the maximum output voltage obtained was 67.534 mV due to the overlapping electric double-layer effect formed by hydrogen protons on the TPPA surface, and the energy utilization efficiency is 95.95%. Moreover, TPPA-5 can purify pesticide-containing wastewater, which has the advantages of being recyclable and environmentally friendly, showing potential application value in the field of seawater desalination and steam co-generation.