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Abstract Lightweight energy storage devices are essential for developing compact wearable and distributed electronics, and additive manufacturing offers a scalable, low‐cost approach to fabricating such devices with complex geometries. However, additive manufacturing of high‐performance, on‐demand energy storage devices remains challenging due to the need for stable, multifunctional nanomaterial inks. Herein, the development of 2‐dimensional (2D) titanium carbide (Ti₃C₂T_xMXene) ink that is compatible with aerosol jet printing for energy storage applications is demonstrated. The developed MXene ink demonstrates long‐term chemical and physical stability, ensuring consistent printability and achieving high‐resolution prints (≈45 µm width lines) with minimal overspray. The high‐resolution aerosol‐jet printed MXene supercapacitor achieves an areal capacitance of 122 mF cm⁻²and a volumetric capacitance of 611 F cm⁻³, placing them among the highest‐performing printed supercapacitors reported to date. These findings highlight the potential of aerosol jet printing with MXene inks for on‐demand, scalable, and cost‐effective fabrication of printed electronic and electrochemical devices. 

Electrospray deposition (ESD) uses strong electric fields applied to solutions and dispersions exiting a capillary to produce charged monodisperse droplets driven toward grounded targets. Self‐limiting electrospray deposition (SLED) is a phenomenon in which highly directed, uniform, and even 3D coatings can be achieved by trapping charge in the deposited film, redirecting the field lines to uncoated regions of the target. However, when inorganic particles are added to SLED sprays, the buildup of charge required to repel incoming material is disrupted as particle loading increases. Due to its fibril gelling behavior, methylcellulose (MC) SLED can form nanowire morphologies. These wires, when used as a binder, can separate particles and prevent percolation. In this work, a variety of conductive and insulating particles are explored using patterned and un‐patterned substrates. This exploration allows us to maximally load particles for high‐concentration and highly controlled self‐limiting functional sprays. This is demonstrated using Ti3C2Tx MXene to functionalize an interdigitated electrode for use as a supercapacitor.