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The increasing demand for higher‐energy‐density batteries driven by advancements in electric vehicles, hybrid electric vehicles, and portable electronic devices necessitates the development of alternative anode materials with a specific capacity beyond that of traditional graphite anodes. Here, the state‐of‐the‐art developments made in the rational design of Si‐based electrodes and their progression toward practical application are presented. First, a comprehensive overview of fundamental electrochemistry and selected critical challenges is given, including their large volume expansion, unstable solid electrolyte interface (SEI) growth, low initial Coulombic efficiency, low areal capacity, and safety issues. Second, the principles of potential solutions including nanoarchitectured construction, surface/interface engineering, novel binder and electrolyte design, and designing the whole electrode for stability are …