Electrostatically Induced Intercalation of Layered Double Hydroxide in Graphene Oxide for Enhanced Electrochemical Energy Storage

Electrostatically intercalated MgAl‐layered double hydroxide (LDH) nanosheets act as non‐redox spacers to prevent rGO restacking via a self‐assembly process. Such layer‐by‐layer structure provides accessible nano‐channels for rapid ion transport, exhibiting high capacitance (410 F g−1) with robust retention and cycling stability. This strategy provides a scalable method of designing the layered 2D materials for next‐generation supercapacitors. Abstract Graphene‐based materials have great potential for electrochemical energy storage applications, but their performance is often limited by the restacking of nanosheets, which restricts ion accessibility. In this study, a straightforward method to fabricate reduced graphene oxide (rGO) laminates intercalated with magnesium–aluminium layered double hydroxide (MgAl‐LDH) nanosheets is presented. Due to electrostatic interactions, the positively charged LDH nanosheets strongly bind to the negatively charged rGO layers, forming a stable, alternating laminar structure with well‐defined nano‐capillaries. Detailed characterization confirms the intended architecture of the rGO‐LDH hybrid. Electrochemical analysis shows nearly ideal electric double‐layer capacitor (EDLC) behavior, with the rGO‐LDH reaching a specific capacitance of up to 410 F g−1 at 1 A g−1. This work highlights the vital role of LDH nanosheets as interlayer spacers that effectively prevent restacking, providing new insights into designing 2D materials for high‐performance supercapacitors and energy storage systems. Electrostatically intercalated MgAl-layered double hydroxide (LDH) nanosheets act as non-redox spacers to prevent rGO restacking via a self-assembly process. Such layer-by-layer structure provides accessible nano-channels for rapid ion transport, exhibiting high capacitance (410 F g −1 ) with robust retention and cycling stability. This strategy provides a scalable method of designing the layered 2D materials for next-generation supercapacitors. Abstract Graphene-based materials have great potential for electrochemical energy storage applications, but their performance is often limited by the restacking of nanosheets, which restricts ion accessibility. In this study, a straightforward method to fabricate reduced graphene oxide (rGO) laminates intercalated with magnesium–aluminium layered double hydroxide (MgAl-LDH) nanosheets is presented. Due to electrostatic interactions, the positively charged LDH nanosheets strongly bind to the negatively charged rGO layers, forming a stable, alternating laminar structure with well-defined nano-capillaries. Detailed characterization confirms the intended architecture of the rGO-LDH hybrid. Electrochemical analysis shows nearly ideal electric double-layer capacitor (EDLC) behavior, with the rGO-LDH reaching a specific capacitance of up to 410 F g −1 at 1 A g −1. This work highlights the vital role of LDH nanosheets as interlayer spacers that effectively prevent restacking, providing new insights into designing 2D materials for high-performance supercapacitors and energy storage systems. Advanced Science, Volume 12, Issue 48, December 29, 2025.