AbstractHyperbolic paraboloid surfaces or saddle‐shaped materials can exist in two equilibrium shapes when the saddle shape reverses on itself and, therefore, can be used as structural elements of new stimuli‐responsive and shape‐changing materials. Here we propose a new fast and easy approach to the nanoarchitectonics of graphene oxide nanosheets to form curved interfaces. Our technology involves computer‐aid design, three dimensional (3D) printing, and casting curved templates for the assembly of two‐dimensional (2D) nanosheets. We demonstrate the feasibility of our approach for the nanoarchitectonics of graphene oxide flakes, though it can be expanded to include the whole family of 2D materials. The prepared free‐standing saddle‐shaped graphene oxide membranes show highly ordered nanostructure, typical for flat 2D multilayered materials. We optimize the preparation conditions to construct robust two‐dimensional membranes with nanostructured architecture and controllable thickness and curvature.