Aerogels have great potential in oil absorption applications; however, many reported aerogels have the drawbacks of a low oil-recovery rate and poor mechanical properties, which limit their application. In this study, highly reusable graphene oxide (GO)/TEMPO-oxidized cellulose nanofiber (TOCN)/polyvinyl alcohol (PVA) aerogels with excellent mechanical properties and with an architecture similar to that of Thalia dealbata stems were fabricated through a three-step process of bidirectional-freezing, freeze-drying, and chemical vapor deposition (CVD) modification. After CVD modification, the modified GTPA (MGTPA) accorded hydrophobicity. The synergistic effects of the three components and the unique biomimetic structure conferred biomimetic-MGTPA (b-MGTPA) with excellent compressible properties. As an adsorbent, b-MGTPA showed a high adsorption capacity (75–151 g/g) for various types of organic solvents. In addition, its high compressibility enables b-MGTPA to have fast and highly efficient recovery of absorbed oil through simple mechanical squeezing and it possesses excellent reusable stability (the oil recovery rate and oil retention rate reached 80% and 91.5%, respectively, after 10 repeated absorption–compression cycles).