To advance the use of electron diffraction methodologies on the study of MOF structure further, we sought to incorporate the use of focused ion beam milling (FIB) under cryogenic temperatures (cryo-FIB) into the MicroED structure determination workflow to control crystal thickness. FIB milling has generally been used in semiconductor manufacturing and materials science for site-specific analysis, deposition, and ablation of materials. The use of FIB milling for sensitive samples is often thought to be too damaging for high-resolution studies. However, recently it has been shown that the use of cryo-FIB milling can facilitate high-resolution imaging of MOF samples up to 1.2 Å . For macromolecular crystallography, coupling cryo-FIB milling of crystals with MicroED analysis for high-resolution structure determination has become a powerful approach, with several recent studies using these methods . However, this approach has not yet been demonstrated for electron diffraction of organic frameworks.