With increasing demands for high energy lithium-ion batteries, layered nickel-rich cathode materials have been considered as the most promising candidate due to their high reversible capacity and low cost. Although some of the materials with nickel contents <= 60 % were commercialized, there are tremendous obstacles for further improvement of electrochemical performance, which is strongly related to the unstable cathode surface and interfacial properties. In this regard, a specific review on the interfacial chemistry between the cathode and electrolyte during electrochemical testing is provided. We highlight the underpinning interfacial chemistry and degradation mechanisms of the cathode materials. Finally, light is shed on the recent efforts for enhancing the interfacial stability of the nickel-rich cathode materials.