Rechargeable lithium‐ion batteries with good electrochemical properties require nanostructured electrode materials, which are usually prepared through complex synthesis processes. Herein, a new facile method is reported for the synthesis of high‐performance electrode materials with a crater‐like morphology through repulsion between positive charges. The produced electrode material does not possess a nanostructure. However, it is capable of rapidly transferring lithium ions and electrons owing to the large contact area with electrolyte and the high concentration sp2‐hybridized carbon coating. LiFePO4 and LiNi1/3Co1/3Mn1/3O2 electrodes prepared by this process achieved high discharge capacities of 165.7 and 199.9 mAh g−1 at 0.1 C, with excellent rate capability of 127.5 and 162.6 mAh g−1 at 10 C, respectively. Although the crater‐type materials might decrease the electrode tap density, they facilitate better electrochemical properties such as high capacity, high power, and fast charging. Furthermore, this new method can be applied trough a sol–gel process for the synthesis of electrode materials to improve their electrochemical characteristics.