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The MXene combining high conductivity, hydrophilic surface, and wide chemical variety has been recognized as a rapidly rising star on the horizon of two-dimensional (2D) material science. However, strong tendency to intersheet aggregate via van der Waals force represents a major problem limiting the functionalities, processability, and performance of MXene-based material/devices. We report a capillary-forced assembling strategy for processing MXene to hierarchical 3D architecture with geometry-based high resistance to aggregation. Aggregate-resistant properties of 3D MXene not only double the surface area without loss of the intrinsic properties of MXene but also render the characteristics such as kinetics-favorable framework, high robustness, and excellent processability in both solution and solid state. Synergistically coupling the 3D MXene with electrochemically active phases such as metal oxide …