In this study a new approach for aerogel preparation is presented, along with the screening of obtained aerogel towards air decontamination potential. The synthesis method allows the tuning of the porosity degree of the aerogel by changing the amount of the solvent (water), which dictates the physical appearance of the obtained aerogel (compacted or expanded). Experiments have been carried out under dynamic conditions, by using isobutylene (ISB) as model pollutant and activated carbon as a reference sorbent. At low contaminant loading, the obtained aerogels exhibit comparable performance with that observed for activated carbon, otherwise the activated carbon presents the highest performance at higher loadings. The physical appearance of the aerogel appears to influence the ISB removal performance. Influence of gas flowrate and ISB concentration on the performance response is depicted. The obtained results reveal new perspectives in developing and using aerogels (ultralight materials) for the removal of air contaminants in special applications such as those related to gas safety (for example, the gas masks that should assure not only quality, but also comfort).