there are only a few reports on 2D LiFePO 4 materials with outstanding high-rate performance and hybrid battery and supercapacitor behavior. [9,[13][14][15] This is due to the fact that transition metals in cathode materials would undergo oxidation to higher valence states on the removal of lithium or other cations, [16] leading to large compositional changes and the consequent phase changes. Therefore, cathode materials require high structural stability to provide a high specific capacity at high charge and discharge rates, as well as suitable morphology and particle size. Nowadays, the challenge is to develop a versatile, scalable, highly efficient process to synthesize 2D cathode nanosheets, which could maintain their stable crystal structure and uniform microstructure over the long run.The current state-of-the-art cathode materials for Li-ion batteries mainly have three different type of structures, including layered (LiCoO 2 , LiNi 1/3 Mn 1/3 Co 1/3 O 2 , LiNiCoAlO 2 ), spinel (LiMn 2 O 4 ), and olivine-type (LiFePO 4 ) structures. (Please see Figure S1, Supporting Information.) Moreover, the diffusion direction of lithium in LiCoO 2 is octahedral site-tetrahedral site-octahedral site in layers, while that in LiMn 2 O 4 is tetrahedral siteoctahedral site-tetrahedral site with 3D channels, and the motion of lithium ions in LiFePO 4 occurs along 1D channels via nonlinear trajectory in the olivine crystal structure. [17] These different structures certainly will increase the difficulty of the synthesis of 2D cathode nanosheets. Thus, it is a challenge to adopt a general process to synthesize their 2D nanosheets from the corresponding particles with different crystal structures. In addition, the storage mechanisms of 2D layered lithium transition metal oxides or spinel LiMn 2 O 4 nanosheets still need investigation.Herein, we used an effective, easily scaled-up, and general synthetic process for the preparation of few-layered positive electrode nanosheets, which include layered LiCoO 2 , olivinetype LiFePO 4 , and spinel-type LiMn 2 O 4 . These prepared nanosheets showed highly oriented facets, which will have benefits for the lithium ion de-insertion/insertion during the charging/discharging process, respectively, thereby delivering high-energy densities and excellent rate capabilities. Also, the structural evolution of 2D cathode materials during galvanostatic charge-discharge was captured using time-resolved in situ synchrotron X-ray powder diffraction. The transport channels of 2D cathode materials would be opened up to different The most promising cathode materials, including LiCoO 2 (layered), LiMn 2 O 4 (spinel), and LiFePO 4 (olivine), have been the focus of intense research to develop rechargeable lithium-ion batteries (LIBs) for portable electronic devices. Sluggish lithium diffusion, however, and unsatisfactory long-term cycling performance still limit the development of present LIBs for several applications, such as plug-in/hybrid electric vehicles. Motivated by the success of graphene and novel 2D m...