This study introduces an effective strategy for hydrophobizing metal-organic frameworks (MOFs) using oleyl phosphate (OP) ligands. This modification makes MOF particles dispersible in nonpolar solvents and provides them with colloidal stability akin to traditional colloidal nanocrystals (NCs). The resulting OP-capped MOF particles can then be employed as building blocks for constructing various two-dimensional (2D) and 3D superlattices through self-assembly methods typically used for NCs. Additionally, binary superlattices with tailored structures can be achieved by coassembling OP-capped MOF particles with different NCs. This robust surface hydrophobization approach is adaptable to various MOFs, facilitating the rational design and creation of complex MOF-based superstructures.