Nonuniform electrodeposition of lithium during charging processes is the key issue hindering development of rechargeable Li metal batteries. This deposition process is largely controlled by the solid electrolyte interphase (SEI) on the metal surface and the design of artificial SEIs is an essential pathway to regulate electrodeposition of Li. In this work, an electro‐chemo‐mechanical model is built and implemented in a phase‐field modelling to understand the correlation between the physical properties of artificial SEIs and deposition of Li. The results show that improving ionic conductivity of the SEI above a critical level can mitigate stress concentration and preferred deposition of Li. In addition, the mechanical strength of the SEI is found to also mitigate non‐uniform deposition and influence electrochemical kinetics, with a Young's modulus around 4.0 GPa being a threshold value for even deposition of Li. By comparison of the results to experimental results for artificial SEIs it is clear that the most important direction for future work is to improve the ionic conductivity without compromising mechanical strength. In addition, the findings and methodology presented here not only provide detailed guidelines for design of artificial SEI on Li‐metal anodes but also pave the way to explore strategies for regulating deposition of other metal anodes.

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