Lithium–sulfur (Li–S) batteries have great promise to support the next‐generation energy storage if their sluggish redox kinetics and polysulfide shuttling can be addressed. The rational design of sulfur electrodes plays key roles in tacking these problems and achieving high‐efficiency sulfur electrochemistry. Herein, a synergetic defect and architecture engineering strategy to design highly disordered spinel Ni–Co oxide double‐shelled microspheres (NCO‐HS), which consist of defective spinel NiCo2O4–x (x = 0.9 if all nickel is Ni2+ and cobalt is Co2.13+), as the multifunctional sulfur host material is reported. The in situ constructed cation and anion defects endow the NCO‐HS with significantly enhanced electronic conductivity and superior polysulfide adsorbability. Meanwhile, the delicate nanoconstruction offers abundant active interfaces and reduced ion diffusion pathways for efficient Li–S chemistry. Attributed to these synergistic features, the sulfur composite electrode achieves excellent rate performance up to 5 C, remarkable cycling stability over 800 cycles and good areal capacity of 6.3 mAh cm−2 under high sulfur loading. This proposed strategy based on synergy engineering could also inform material engineering in related energy storage and conversion fields.

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