Li‐rich Mn‐based layered oxides are regarded as the most promising cathode materials for advanced lithium‐ion batteries with energy density as high as 400 Wh kg−1. However, decline of capacity and discharge potential derived from phase transformation during cycling is still an obstacle for practical utilization of Li‐rich cathode materials. Undoubtedly, an in‐depth understanding origin and evolution of the phase transformation from bottom to top is crucial to solve the problem finally. Herein, the recent representative progress on Li‐rich cathode materials from top to bottom is summarized: starting from relationship between dimensions and performance, to evolution of phase transformation, finally to participation of anions during charge–discharge cycling. It systematically shows what happens in the different microscopic levels and how these phenomena relate to cycling of Li‐rich cathode materials with the help of emerging state‐of‐the‐art characterization techniques. On the basis of this progress, it is proposed that rational structural design can fully play its role to build high‐performance energy storage materials and enhance structural stability. Recent research progress in Li‐rich Mn‐based layered cathode materials are summarized from dimension–performance relationship to evolution of phase transformation, and to participation of anions during cycling, showing systematically what happens in the different microscopic levels and how these phenomena relate with cycling performance.