storage systems, and electric vehicles. [1][2][3] Accordingly, markets for the conventional secondary battery, energy storage, and transportation have been rapidly increased since last few decades. On the current trends, lithium (Li)-ion batteries (LIBs) dominate the battery market due to their high energy density and extraordinarily long cycle life. [4,5] A cathode active material seems to be a pivotal component of LIBs because it mainly governs the battery electrochemical performance and takes a big portion of the battery price. [6][7][8][9][10] Figure 1 shows the advances in the research on cathode materials. [11][12][13][14][15][16][17][18][19][20] Previous research on LIB cathodes can be divided into three categories: 1) the development of a cathode material with a new chemical composition; 2) the investigation of the material degradation mechanisms; and 3) the modification and improvement of the material performance. [21][22][23][24][25] These three research categories have directly and indirectly influenced one another, leading to further progress and advance of LIBs.Controlling chemical composition has been considered as one of the most feasible methods not only for the development of new materials but also for the modification and improvement of the structural stability of layered-structured cathode materials. [1,26] By optimizing the active material composition with transition metals (TMs), various candidates for electric vehicles and in the energy storage market have been screened and identified. However, the previous doping research frequently focused on the bulk properties of materials. Particularly, optimizing TM composition and structure was of interest, instead of in-depth investigation into their properties at the atomic level, which was presumably attributed to a lack of advanced research instruments.Recently, the development of analysis equipment and methods with atomic resolution such as transmission electron microscopy (TEM) or X-ray absorption near-edge structure (XANES) has made a remarkable progress in the research on cathode materials. Advances of TEM enables direct observation of lattice and morphology of lithiated and delithiated electrode materials at both micro and nano levels (TEM). [27][28][29][30][31][32][33] Through the time-of-flight secondary ion mass spectrometry analysis, in-depth research of Li-related components on the surface of electrode materials can be studied. [34,35] Furthermore, the development of new X-ray techniques has opened the investigation of fine structure of the electrode materials. For instance, X-ray absorption spectroscopy This work not only summarizes the previous doping research that focused on the optimization of a bulk doping composition but also introduces a new doping strategy, namely, "electrochemical reaction mechanism control doping." The new electrochemical mechanism control technology enables the study of the precise deterioration mechanism of layered cathode materials for Li-ion batteries (LIBs). Accordingly, tremendous efforts have been devote...