The aggressive consumption of fossil fuels has resulted in the uncontrolled release of greenhouse gases such as carbon dioxide and methane into the atmosphere, trapping heat and causing havoc to the environment. With this in mind, the development of sustainable energy is imperative. Renewable energy will fail to reach the anticipated impact unless more efficient way to store and use electricity is found. Therefore, high-performance energy-storage devices with high energy and power density are required for renewable energy sustainability and storage security. Electrochemical batteries have been long considered as one of the most qualified candidates for providing reliable energy storage. Taking into account the safety, power density, cost, longevity and efficiency, rechargeable lithium-ion batteries (LIBs) are the most successful electrochemical storage systems available. The extensive Lithium-ion batteries (LIBs) have become one of the most prevailing techniques for rechargeable batteries. Lithium transition metal oxides are prevalent cathode materials currently, but they face great challenges due to unsatisfactory energy density, chemical/electrochemical instability, and elemental scarcity concerns. Surface/subsurface is the interface where lithium ions cross between the electrolyte and the cathode materials. Its properties and complicated nature are unambiguously regarded as a crucial controlling factor for the overall performance. Tremendous efforts have been made in the exploration of surface modification methods with remarkable progress hitherto. The purpose of this work is to review these surface behaviors in order to understand their fundamental origins and provide a summary of various surface modification methods that can be used to address impeding issues. Finally, a rational method of surface modification is proposed for use in cathode materials.