For suitability in thermal catalysis, a MOF must be stable at high temperatures. The average thermal decomposition temperature from the experimental thermogravimetric analysis (TGA) dataset used to train the thermal stability ANN was 359°C, which corresponds to the lower limit of decomposition temperatures for stable MOFs. Chemical heuristics, confirmed by analysis of synthesized MOFs, tell us that the most thermally stable MOFs do not contain 3d transition metals. We sought MOFs that contain first-row transition metals with moderate thermal stability for catalytic applications and used a thermal decomposition temperature cutoff of 300°C, which narrowed our dataset to 733 MOFs. Although the decomposition temperature from a TGA measurement may be expected to be an overestimate of the temperature at which the material may break down during catalytic conditions, our use of a relatively high cutoff for thermal stability should still yield MOFs with stabilities suitable for catalysis at elevated (e.g., 200 °C) temperatures. Retaining only MOFs with confidently predicted stability by applying uncertainty quantification metrics to ANN predictions, our dataset was reduced to 334 MOFs, 58% of which had an experimental ground truth from the TGA dataset and 54% were unseen by ANN thermal model training data (i.e., because they were unavailable or were in the test partition, Supporting Information Table ). Next, we identified MOFs with identical metal-centered RACs as these would have equivalent metal-coordination environments (Figure ). We retained only the MOF with the highest decomposition temperature prediction for MOFs with identical metal coordination environments to avoid redundant calculations on MOF SBU cluster models, reducing our data set to 184 MOFs (Figure ). Next, we used MOFSimplify to extract the SBUs from their periodic structures and computed atomic-weighted molecular graph determinants of each extracted SBU to retain a single copy of each unique SBU for each MOF (i.e., as judged by connectivity), with the 184 MOFs yielding 242 unique SBUs (Figure ). We expect that a metal site in an SBU can only be catalytically active for methane to methanol catalysis if it has an open metal site (i.e., for a 3d transition metal, the coordination number cannot exceed five). We computed the coordination number of each metal site across all 242 SBUs, automatically categorizing metal sites with coordination numbers 2 and 3 as having open sites. Because metal sites with coordination numbers 4 or 5 are "open" only for certain geometries, we performed a geometry index analysis and used heuristic cutoffs to identify open sites (Supporting Information Figure ). Our workflow retained SBUs with at least one open metal site available for reactivity (Figure ). We studied the formation of a terminal metal-oxo species at the open metal site because these have been found to be capable of C-H activation, but SBUs with multiple metal centers that have strong metal-metal interactions could favor formation of other metal-oxygen species (e.g., bridged µ-metal-oxo). To reduce the likelihood of identifying SBUs with these preferred intermediates, we computed formal shortness ratios (FSR) for all possible pairs of metals in each SBU with more than one metal site (Supporting Information Figure ). We eliminated SBUs with a FSR of < 1.1, which is a conservative threshold for identifying SBUs with strong metal-metal interactions. This results in 144 SBUs corresponding to 110 MOFs with open metal sites capable of terminal metal-oxo formation (Figure ). Lastly, we applied two additional filters in our MOF screening workflows based on practical considerations. We eliminated MOFs that have poor crystal quality 87 as well as MOFs containing halogens bound to the linker or SBU (Figure and Supporting Information Text S1). Therefore, our final data set comprised 101 CoRE MOFs (135 SBUs) that are stable and have potential to be repurposed for methane to methanol catalysis.