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The effectiveness of using catalyst nanoparticles to reduce the overpotential and energy efficiency of lithium–oxygen (or lithium–air) batteries (LOBs) is usually attributed to the inherent catalytic properties of individual nanoparticles. Here, we demonstrate that the morphology of the catalyst layer is equally important in maintaining integrity of the catalyst coating during product formation in LOBs. We demonstrate this by comparing the performance of smooth, conformal coated Mn2O3 catalyst nanoparticles prepared by electric field-assisted deposition, and more irregular coatings using conventional film assembly techniques both on three-dimensional mesh substrates. Smooth coatings lead to an improved overpotential of 50 mV during oxygen reduction and 130 mV during oxygen evolution in addition to a nearly 2X improvement in durability compared to the more irregular films. In situ electrochemical impedance spectroscopy combined with imaging studies elucidates a mechanism of morphology-directed deactivation of catalyst layers during charging and discharging that must be overcome at practical electrode scales to achieve cell-level performance targets in LOBs. [ABSTRACT FROM AUTHOR]