A Li-air battery could potentially provide three to five times higher energy density/specific energy than conventional batteries and, thus, enable the driving range of an electric vehicle to be comparable to gasoline vehicles. However, making Li-air batteries rechargeable presents significant challenges, mostly related to the materials. Here, the key factors that influence the rechargeability of Li-air batteries are discussed with a focus on nonaqueous systems. The status and materials challenges for nonaqueous rechargeable Li-air batteries are reviewed. These include electrolytes, cathode (electrocatalysts), lithium metal anodes, and oxygen-selective membranes (oxygen supply from air). A perspective for the future of rechargeable Li-air batteries is provided.