We use quantized molecular dynamics simulations to investigate the competition between concerted and sequential proton-coupled electron-transfer (PCET) reaction mechanisms in inorganic catalysts. By analyzing reactive nonadiabatic PCET trajectories and computing both concerted and sequential rate constants, we characterize various molecular features that govern inorganic PCET reactions, including the solvent polarity, ligandmediated electron proton interactions, and intrinsic proton transfer (PT) energy barrier. Using atomistic simulations with over 1200 atoms, we find that the symmetric iron biimidazoline system is extremely biased toward the concerted mechanism because of the strong ligand-mediated electron proton interaction and the short PT distance. However, by investigating system bath models in which electron proton interactions are shielded, which are representative of ruthenium terpyridylbenzoates and iron (tetraphenylporphyrin)-benzoates, we predict that a crossover between the concerted and sequential PCET mechanisms may be possible either by increasing the polarity of the solvent or by increasing the intrinsic PT energy barrier. In addition, we predict the possibility of a crossover in the PCET mechanism by directly varying the strength of the ligand-mediated electron proton interactions. The results presented here reveal new strategies for altering the competition between the competing PCET mechanisms and design principles for controlling PCET in catalytic systems.