Rational construction of sulfur electrodes is essential in pursuit of practically viable lithium-sulfur (Li-S) batteries. Herein, bimetallic NiCo-layered double hydroxide (NiCo-LDH) with a unique hierarchical micro-nano architecture is developed as an advanced sulfur reservoir for Li-S batteries. Compared with the monometallic Co-layered double hydroxide (Co-LDH) counterpart, the bimetallic configuration realizes much enriched, miniaturized, and vertically aligned LDH nanosheets assembled in hollow polyhedral nanoarchitecture, which geometrically benefits the interface exposure for host-guest interactions. Beyond that, the introduction of secondary metal intensifies the chemical interactions between layered double hydroxide (LDH) and sulfur species, which implements strong sulfur immobilization and catalyzation for rapid and durable sulfur electrochemistry. Furthermore, the favorable NiCo-LDH is architecturally upgraded into closely packed micro-nano clusters with facilitated long-range electron/ion conduction and robust structural integrity. Due to these attributes, the corresponding Li-S cells realize excellent cyclability over 800 cycles with a minimum capacity fading of 0.04% per cycle and good rate capability up to 2 C. Moreover, highly reversible areal capacity of 4.3 mAh cm −2 can be achieved under a raised sulfur loading of 5.5 mg cm −2. This work provides not only an effective architectural design but also a deepened understanding on bimetallic LDH sulfur reservoir for high-performance Li-S batteries.

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Lithium–sulfur (Li–S) batteries present a promising solution to high‐energy and low‐cost energy storage. However, the conversion‐type redox mechanism determines the poor fulfillment of battery chemistry in terms of reversibility and kinetics. Herein, a flower‐like graphene microassembly decorated with finely‐dispersed Ni2Co nanoalloy (Ni2Co@rGO) is developed as advanced host matrix for Li–S batteries. Combining computational, physicochemical, and electrochemical studies, Ni2Co nanoalloys are unveiled synergizing strong adsorbability against polysulfide shuttling and excellent catalytic activity for sulfur conversions. Meanwhile, the sophisticated architecture renders facile electron/ion transport and highly‐exposed active interfaces. These virtues collaboratively contribute to fast and durable sulfur electrochemistry with a minimum capacity degradation of 0.034% per cycle over 500 cycles and a rate capability up to 5 C. Besides, the implementation of Ni2Co@rGO as the anode matrix tames the Li redox behavior benefiting from the enhanced lithiophilicity and reduced local current density. As such, the full cell configuration pairing S‐Ni2Co@rGO cathode and Li‐Ni2Co@rGO anode realizes a favorable areal capacity of 4.53 mAh cm−2 under high sulfur loading (4.0 mg cm−2) and limited electrolyte (E/S = 6.0 mL g−1). This work offers an elaborate bi‐service matrix engineering to simultaneously improve the conversion reversibility and kinetics for superior Li–S batteries.

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