Herein, we present a facile strategy to prepare versatile aluminum oxide subnanometer nanosheets with oleic acid and stearic acid ligands (OA-Al SNSs and SA-Al SNSs, respectively). The size effect endows subnanosheets with abundant acting sites, remarkable intermolecular interactions, and unique polymer-like properties, including flexibility, viscoelasticity, and sol−gel transitions, which is quite different from traditional inorganic materials. Consequently, subnanosheets could form freestanding organogels and OA-Al SNSs exhibit satisfying semisolidification of various solvents, making it an intriguing candidate for the safe storage and transportation of solvents. Furthermore, SA-Al SNSs exhibit excellent adhesive properties of high strength on diverse substrates, and it is easy to erase it without any damage, demonstrating the promising prospects in practical applications.