Metal-organic frameworks (MOFs) are a class of porous materials known for high surface area as well as highly tunable porous structures, topologies, and functionalities. They are synthesized by the coordination of a metal or metal oxide node with an organic linker. The relative ease of synthesis and the degree of tunability have made MOFs a material of choice for diverse applications including gas storage and separations, 5, 6 sensing, 7, 8 catalysis, and biochemical applications. While most MOFs have threedimensional (3D) morphology, several MOFs have been reported in two-dimensional (2D) and thin platelet morphologies. 2D MOFs are synthesized in lamellar sheets, where it has been shown that these layers can be exfoliated into monolayers which are attractive as a building block of thin films. UiO-66, named after the University of Oslo, is one of the most studied MOFs thanks to its exceptional chemical and thermal stability attributed to a strong Zr-O bond and a high coordination number of Zr. UiO-66 is formed by the coordination of zirconium-oxo cluster with terephthalic acid where an octahedral cage shares its eight triangular faces with eight tetrahedral cages (Figure ), each featuring a Å-scale triangular aperture. The pore size of UiO-66 is attractive to differentiate molecules and ions. Thanks to its high stability including in water, UiO-66 films have been explored for gas separation, desalination, and ion-ion separation. UiO-66 possesses a 3D structure. Its synthesis in 2D morphology has not been reported mainly because of the challenges from the isotropic robust bonds in its structure. While an emerging class of non-van der Waals (non-vdW) quasi-2D materials has been synthesized from non-layered 3D crystals, they have been predominantly demonstrated for transition metal oxides. Extending this concept to MOFs, and in particular UiO-66, is highly attractive to prepare 2D morphologies and ultrathin films for advancing thin film applications for highly stable MOFs. A potential approach is anisotropic 2D growth of UiO-66, however, this has not been reported. As a result, the state-of-the-art UiO-66 films are 2-3 orders of magnitude thicker than the desired 2D film (Figure and Table ).