For assembly, a purified amphiphilic polypeptoid of specific sequence is dissolved in aqueous solution. These form a monolayer (Langmuir–Blodgett film) on the air-water interface with their hydrophobic side chains oriented in air and hydrophilic side chains in the water. When this mono-layer is shrunk, it buckles into a bilayer with the hydrophobic groups forming the interior core of the peptoid nanosheet. This method has been standardized in the Zuckermann laboratory by repetitively tilting vials of peptoid solution at 85° before returning the vials to the upright position. This repetitive vial “rocking” motion lessens the interfacial area of the air-water interface inside the vial, compressing the peptoid mono-layer by a factor of four and causing the mono-layer to buckle into peptoid nanosheets. Using this method, nanosheets are produced in high yield, and 95% of the peptoid polymer starting material is efficiently converted into peptoid nanosheets after rocking the vials several hundred times.