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Manufacturing of printed electronics relies on the deposition of conductive liquid inks, typically onto polymeric or paper substrates. Among available conductive fillers for use in electronic inks, carbon nanotubes (CNTs) have high conductivity, low density, processability at low temperatures, and intrinsic mechanical flexibility. However, the electrical conductivity of printed CNT structures has been limited by CNT quality and concentration, and by the need for nonconductive modifiers to make the ink stable and extrudable. This study introduces a polymer‐free, printable aqueous CNT ink, and, via an ambient direct‐write printing process, presents the relationships between printing resolution, ink rheology, and ink‐substrate interactions. A model is constructed to predict printed feature sizes on impermeable substrates based on Wenzel wetting. Printed lines have conductivity up to 10 000 S m −1 . The lines are flexible, with <5% change in DC resistance after 1000 bending cycles, and <3% change in DC resistance with a bending radius down to 1 mm. Demonstrations focus on i) conformality, via printing CNTs onto stickers that can be applied to curved surfaces, ii) interactivity using a CNT‐based button printed onto folded paper structure, and iii) capacitive sensing of liquid wicking into the substrate itself. Facile integration of surface mount components on printed circuits is enabled by the intrinsic adhesion of the wet ink.

Substrate‐Versatile Direct‐Write Printing of Carbon Nanotube‐Based Flexible Conductors, Circuits, and Sensors