We developed a HTVS workflow to guide the systematic discovery of MOF catalysts for the conversion of methane to methanol from a diverse space of materials. Unlike previous workflows, our approach mandated both MOF stability and synthesizability while identifying MOFs with promising unsaturated metal sites (i.e., Mn, Fe, Co, or Cu) amenable to forming a terminal metal-oxo for C-H activation. To determine which of our materials were candidate catalysts, we carried out DFT calculations on 87 selected MOFs to determine methane-to-methanol reaction energetics following the radical rebound mechanism. Despite significant metal-local structural diversity in our MOFs, formation of oxo intermediates becomes less favorable with increasing 3d filling, as observed in octahedral metal complexes. At odds with prior work, our diverse set indicates opportunities to disrupt scaling limitations between oxo formation and HAT.