Fungicide contamination is a critical environmental issue, and the effective removal of fungicide residues from aquatic environments has attracted significant attention from researchers. In this study, the synthesized hyperbranched polysiloxane (TA-HBPSi) was grafted onto TEMPO-oxidized cellulose nanofibers (TOCNF) to fabricate a novel aerogel material (TA-HBPSi@TOCNF) with the aim of enhancing the sorption efficiency of fungicide. The equilibrium maximum adsorption capacity of TA-HBPSi@TOCNF for imazalil (8.04 mg/g) was significantly higher compared to other fungicides, including prochloraz (6.43 mg/g), thiophanate-methyl (4.12 mg/g), carbendazim (0.16 mg/g), and thiabendazole (0.04 mg/g). In the presence of Cd