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Abstract Practical applications of lithium metal batteries are often limited by low cycling efficiencies and uncontrolled lithium dendrite growth caused by unstable and heterogeneous lithium‐electrolyte interfaces. To address this issue, a calix[4]pyrrole‐based wavy covalent organic framework (WCOF) is developed that acts as a protective layer to suppress Li dendrite growth and reduce side reactions on the Li anode. The presentWCOFis porous and contains calix[4]pyrrole units acting as “molecular traps” that allow efficient PF₆⁻anion capture while allowing for uniform Li⁺diffusion. This provides structurally stable artificial protective layers that permit high Li⁺transference numbers. The resulting solid electrolyte interphases permit ultralong‐term stable cycling at a current density of 1 mA cm⁻²and reversible lithium plating/stripping (over 2500 h) at an areal capacity of 2 mAh cm⁻². The protected anodes of this study also demonstrated excellent cell stability through 260 cycles when paired with high‐voltage cathodes (NCM811 with high mass loading: 20 mg cm⁻²). 

A review highlights improvements in synthesizing and stabilizing multielement nanoparticles. 

Multi-principal element intermetallic nanoparticles are synthesized via disorder-to-order transition.