The rapid development of miniaturized electronic devices has greatly stimulated the endless pursuit of high-performance on-chip micro-supercapacitors (MSCs) delivering both high energy and power densities. To this end, an advanced three-dimensional (3D) microelectrode architecture design offers enormous opportunities due to high mass loading of active materials, large specific surface areas, fast ion diffusion kinetics, and short electron transport pathways. In this review, we summarize the recent advances in the rational design of 3D architectured microelectrodes including 3D dense microelectrodes, 3D nanoporous microelectrodes, and 3D macroporous microelectrodes. Furthermore, the emergent microfabrication strategies are discussed in detail in terms of charge storage mechanisms and structure− performance correlation for on-chip MSCs. Finally, we conclude with a perspective on future opportunities and challenges in this thriving field.

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Hybrid composite electrolytes incorporate polymer matrixes and garnet filler attract the focus of concern for all‐solid‐state batteries, which possess high ionic conductivity, superior electrochemical stability, and wide electrochemical window of ceramic electrolyte advantages, and exhibit excellent flexibility and tensile shear strength from polymer electrolyte benefits. Hence, the unique structure design of solid‐state electrolytes resolves the existing defects that the use of either single garnet or polymer electrolytes implemented into battery devices. This review summarizes Li7La3Zr2O12 (LLZO)/polymer solid composite electrolytes (SCEs), comprising LLZO/polymer SCEs with various structures and different ratios of LLZO fillers, LLZO/polymer with different kinds of polymers matrix and hybrid lithium‐salt, and Li+ transport pathways within the LLZO/polymers SCEs interface. The purpose here is to propose the viewpoints and challenges of LLZO/polymer SCEs to promote the development of next‐generation solid electrolytes.

Abstract2D layered FePS3 is an anode material with high energy density for lithium‐ion batteries. Here, a simple and effective vacuum filtration method is used to successfully synthesize nanocellulose (NC) and FePS3 into a FePS3‐NC electrode with a 3D network structure. Based on the detailed structural characterization, electrochemical testing, and density functional theory, the relationship between NC and FePS3 materials in the lithium storage process is established from the perspective of lithium ions dynamics. The results display that NC can effectively decrease the adsorption energy of FePS3 materials, promote the construction of a 3D network structure, and form flexible FePS3‐NC electrodes. In addition, the migration path of lithium ions in the FePS3‐NC system is more inclined to the Y‐axis, and the migration barrier is also significantly reduced from 0.7714 to 0.4245 eV, which significantly improves the migration speed of lithium ions and the battery capacity. Therefore, the results of this study are conducive to further understand the dynamic mechanism of NC promoting rapid lithium storage in FePS3 materials and can provide good guidance for the study of flexible electrodes.