In this article, we have reviewed our work on understanding and mitigating some of the key factors that limit non-aqueous Li-air battery performance. Advances in Li-air battery technology require fundamental understanding of the discharge and charge processes. We first summarize an investigation of Li-air batteries based on a well-defined cathode surfaces having size-selected silver clusters. This work provided key insight into the nucleation and growth mechanism of the discharge product and its relationship to lowering charge potentials. We then describe the development of new cathode materials including ones based on Pd and Mo2C nanoparticles that give very low charge potentials. This work has shown that it is possible to achieve very good round-trip efficiencies as well as up to 100 cycles in a Li-air cell. Finally, we discuss investigations of likely sources of electrolyte decomposition at the cathode and anode, which need to be resolved in order to achieve the long cycle life that is necessary to enable Li-air batteries. (C) 2015 The Electrochemical Society. All rights reserved.