In some embodiments, the present invention provides amphiphilic nanosheets that comprise lamellar crystals with at least two regions: a first hydrophilic region, and a second hydrophobic region. In some embodiments, the amphiphilic nanosheets of the present invention also comprise a plurality of functional groups that are appended to the lamellar crystals. In some embodiments, the functional groups are hydrophobic functional groups that are appended to the second region of the lamellar crystals. In some embodiments, the lamellar crystals comprise α-zirconium phosphates. Additional embodiments of the present invention pertain to methods of making the aforementioned amphiphilic nanosheets. Such methods generally comprise appending one or more functional groups to a stack of lamellar crystals; and exfoliating the stack of lamellar crystals for form the amphiphilic nanosheets.