Assembling 2D materials such as MXenes into functional 3D aerogels using 3D printing technologies gains attention due to simplicity of fabrication, customized geometry and physical properties, and improved performance. Also, the establishment of straightforward electrode fabrication methods with the aim to hinder the restack and/or aggregation of electrode materials, which limits the performance of the electrode, is of great significant. In this study, unidirectional freeze casting and inkjet‐based 3D printing are combined to fabricate macroscopic porous aerogels with vertically aligned Ti3C2Tx sheets. The fabrication method is developed to easily control the aerogel microstructure and alignment of the MXene sheets. The aerogels show excellent electromechanical performance so that they can withstand almost 50% compression before recovering to the original shape and maintain their electrical conductivities during continuous compression cycles. To enhance the electrochemical performance, an inkjet‐printed MXene current collector layer is added with horizontally aligned MXene sheets. This combines the superior electrical conductivity of the current collector layer with the improved ionic diffusion provided by the porous electrode. The cells fabricated with horizontal MXene sheets alignment as current collector with subsequent vertical MXene sheets alignment layers show the best electrochemical performance with thickness‐independent capacitive behavior.

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In this study, we overviewed the magnetic aerogel for the first time in terms of their major types and important applications, and have paved the way for the further research on this futuristic advanced material.