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To satisfy the functional requirements for next‐generation electronic and optoelectronic devices, diverse protocols have thus been developed for preparing transparent flexible electrodes (TFEs) of metallic nanowires with high flexibility and conductivity, while flexible electrodes with 3D configuration have become a burgeoning frontier. Herein, an innovative 3D network of silver nanorod–nanoparticle hybrids (Ag NNH) is realized by a facile aerosol jet printing (AJP) technique. A dynamic assembly mechanism based on the AJP of silver nanowires (AgNWs) ink is proposed, suggesting a favorable evaporation‐induced migration and assembly process along with the coalescence of deposited droplets. The initially formed Ag NNH random network optimizes the wettability, spreading, and pinning of the droplets, shaping the consecutive deposition behavior of the aerosol droplets for constructing the 3D Ag NNH networks. Planar micro‐supercapacitor (MSC) devices are developed using the Ag NNH network as flexible microelectrode, and a competitive areal capacitance performance has been demonstrated in comparison with other Ag‐based devices. It is envisioned that the as‐developed approach will provide an optional approach for developing future electronic and optoelectronic devices with fascinating hierarchical features. [ABSTRACT FROM AUTHOR]

2D MXene has attracted tremendous attention for developing high‐performance energy storage devices regarding its good metallicity and relatively large accessible surface area. However, the electrochemical performance of MXene‐related devices was hindered due to the pronounced self‐stacking characteristic of MXene. Herein, a convenient aerosol jet printing (AJP) process is developed for the synthesis of MXene nanospheres with crumpled and eccentric structures by modulating the migration and assembly of MXene nanosheets on heat substrate. The existing temperature gradient between the apex and the edge of the deposited droplet causes thermocapillary flows carrying MXene nanosheets toward the edge and the MXene nanosheets are further shaped and assembled along the droplet surface during the solvent evaporation. Interdigital microelectrodes of crumpled MXene nanospheres are tentatively developed for electrochemical performance characterization, a competitive areal capacitance performance is demonstrated in comparison with other MXene‐based devices. Importantly, this work highlights the great potential of the AJP technique for developing functional devices with fascinating hierarchical features as well as further extending applications in miniaturized and intelligent microelectronics. [ABSTRACT FROM AUTHOR]