Rapid extraction and concentration systems based on green materials such as cellulose or lignin are promising. However, there is still a need to optimize the material properties and production processes. Unlike conventional cellulose or lignin sorbent materials, aquatic reed root cells can concentrate external organic pollutants in the water and accumulate them in the plant. Inspired by this, a new nanocellulose-lignin aerogel (NLAG) was designed, in which nanocellulose was used as a substrate and lignin and polyamide epoxy chloropropane were used to crosslink cellulose in order to enhance the strength of the NLGA, resulting in good mechanical stability and water-oil amphiphilic properties. In practical applications, the organic membrane on the NLAG can transport organic pollutants from water to the NLAG, where they are immobilized. This is evidenced by the fact that the aerogel can remove more than 93% of exogenous phenol within a few minutes, highly enriching it inside. In addition, the aerogel facilitates filtration and shape recovery for reuse. This work establishes a novel biopolymer-aerogel-based extraction system with the advantages of sustainability, high efficiency, stability, and easy detachability, which are hard for the traditional adsorbent materials to attain.