This review reports on the most updated technological aspects of Li-air battery cathode materials. It provides the reader with recent developments, alongside critical views. The requirements for air-cathodes, as well as the classification and characterization of carbon-based and carbon-free air cathodes, are listed. The effects of two major substituent groups of materials, namely carbon and advanced materials (metals, metal-oxides, metal-carbides, and metal-nitrides) aimed at replacing carbon, are discussed in terms of their chemical and electrochemical stability. The report covers aspects of surface chemistry and structure influence on the electrolyte and discharge products stability. The review also reports on the efforts to suppress side reactions and deterioration of the polymeric binders (if a composite electrode is being considered). This is recognized as a means to enhance Li-air battery performance. The report concludes with an outlook and perspective, providing the readers with some insight on other factors and their impact on the long road toward a viable air-cathode suitable for Li-air battery operations.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adfm.201808303.respectively. [1] The configuration of an aprotic LOB is based on coupling lithium metal anode and air-breathing cathode in a non-aqueous electrolyte system. The electrochemical reactions occurring during discharge are complex multistep reactions and may involve dissolved and/or adsorbed species alongside parasitic reactions. [2][3][4][5] Oxygen reduction reaction during discharge largely depends on the cathode and electrolytes characteristics; yet, a dominant process involving a two-electron oxygen reduction reaction (ORR), with the formation of Li 2 O 2 , is reported, according to the following reaction [6] The reverse process, namely lithium peroxide oxidation, occurs upon charging. The formation/decomposition of Li 2 O 2 during discharge/charge is often accompanied by parasitic side reactions, due to instability of the major battery components (cathode, electrolyte, and anode) under operating conditions. [7][8][9][10][11][12] While lithium metal anode corrosion can be mitigated by a protective solid electrolyte (SE) membrane, [13][14][15] the electrolyte and cathode are considered as the most challenging components of LOB. Much efforts have been placed on understanding the role of the electrolyte, its degradation, on Li-O 2 reaction mechanism and battery performance. [16][17][18][19][20] Nonetheless, the high discharge/ charge overpotential and severe capacity loss in the course of cycling are also largely related to the air-breathing cathode. A stable, high surface area, cost-efficient air-electrode with excellent catalytic activities toward oxygen reduction and oxidation is crucial for the development of practical LOB. Cathode materials should be stable, durable, and hold interfaces with minimum surface oxide layers, which can inhibit charge transfer during the charging p...