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• Aerogel developed from CNF anchored with transition metal divalent ions enhanced by CNT. • Efficiently absorb ammonia, trimethylamine, hydrogen sulfide, and methyl mercaptan. • The hybrid aerogel showed steady performance in a wide range of temperatures from 0 °C to 40 °C. • The first aerogel type deodorizer material ever reported in air decontamination. • Aerogel is eco-friendly and economic, suitable for domestic and industrial uses. A novel deodorizer that is capable of selectively eliminating the odorous chemicals, such as ammonia, trimethylamine, hydrogen sulfide and methyl mercaptan, is described. The deodorizer is a nanostructured aerogel by nature, consisting of 2,2-6,6-tetramethylpiperidine-1-oxyl (TEMPO) oxidized cellulose nanofibrils (CNF), transition metal divalent cations (M2+), and multi-walled carbon nanotubes (CNT) as the constitutive elements. CNF are firstly mixed with M2+ (M2+, in this paper, typifies Ni2+, Co2+ and Cu2+) to form CNF-M2+ complexes, monodispersed CNT is then mixed to prepare CNT/CNF-M2+ waterborne slurries; CNT/CNF-M2+ hybridized aerogels are finally obtained via freezing-drying of the CNT/CNF-M2+ waterborne slurries. The CNT/CNF-M2+ aerogels are a foam-like structure consisting of CNF and CNT as backbones and M2+ as linkers. The aerogels show higher capabilities (in comparison with activated carbon) for selectively adsorbing ammonia, trimethylamine, hydrogen sulfide and methyl mercaptan. Computing simulations suggest a theoretical conclusion that the odorous chemicals are absorbed in a preferring manner of bimolecular absorptions via the M2+ moieties. The CNT/CNF-M2+ hybridized aerogels are lightweight, eco-friendly, and easy to produce in industrial scales. Our new finding, as is described in this paper, demonstrates potential applications of the TEMPO-oxidized CNF to the field of deodorizations. [ABSTRACT FROM AUTHOR]