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Fabricating complex structures on micro‐ and mesoscales is a critical aspect in the design of advanced sensors and soft electronics. However, soft lithographic methods offer an important approach to fabricating such structures, the progress in the field of additive manufacturing (e.g., 3D printing) offers methods of fabrication with much more material complexity. The rheological complexity of the printing material, however, often dictates the limitations of printing. In particular, the challenges involved in synthesizing printing materials that can enable shape retention at smaller scales (<100 μm), yet be conductive, limits many applications of 3D printing to soft microelectronics. Herein, a printing‐centered approach using a novel particle‐free conductive emulsion ink is presented. This approach separates the printing and polymerization of a conductive monomer (pyrrole) and renders a novel ink that is used to print filaments with heretofore impossible to realize 3D feature dimensions and build structures with high shape retention. The printability of the ink is evaluated, and post‐treatment properties assessed. Multidirectional strain sensors are printed using the emulsion ink to illustrate an exemplary application in soft electronics. 

Abstract The ability to manufacture highly intricate designs is one of the key advantages of 3D printing. Achieving high dimensional accuracy requires precise, often time‐consuming calibration of the process parameters. Computerized feedback control systems for 3D printing enable sensing and real‐time adaptation and optimization of these parameters at every stage of the print, but multiple challenges remain with sensor embedment and measurement accuracy. In contrast to these active control approaches, here, the authors harness frontal polymerization (FP) to rapidly cure extruded filament in tandem with the printing process. A temperature gradient present along the filament, which is dependent on the printing parameters, can impose control over this exothermic reaction. Experiments and theory reveal a self‐regulative mechanism between filament temperature and cure kinetics that allows the frontal cure speed to autonomously match the print speed. This self‐regulative printing process rapidly adapts to changes in print speed and environmental conditions to produce complex, high‐fidelity structures and freestanding architectures spanning up to 100 mm, greatly expanding the capabilities of direct ink writing (DIW).