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Surface patterning of liquid metals (LMs) is a key processing step for LM‐based functional systems. Current patterning methods are substrate specific and largely suffer from undesired imperfections—restricting their widespread applications. Inspired by the universal catechol adhesion chemistry observed in nature, LM inks stabilized by the assembly of a naturally abundant polyphenol, tannic acid, has been developed. The intrinsic adhesive properties of tannic acid containing multiple catechol/gallol groups, allow the inks to be applied to a variety of substrates ranging from flexible to rigid, metallic to plastics and flat to curved, even using a ballpoint pen. This method can be further extended from hand‐written texts to complex conductive patterns using an automated setup. In addition, capacitive touch and hazardous heavy metal ion sensors have been patterned, leveraging from the synergistic combination of polyphenols and LMs. Overall, this strategy provides a unique platform to manipulate LMs from hand‐written pattern to complex designs onto the substrate of choice, that has remained challenging to achieve otherwise.

Liquid metals can play an essential role in the generation of electrically conductive composites for electronic devices and environmental sensing and remediation applications. Here, a method for growing a polyaniline nanofibrous network at liquid metal nanoparticle interfaces is demonstrated for generating hybrid liquid metal–polymer nanocomposites. The investigation shows that an initial functionalization step of the liquid metal nanoparticles with a polymerization enhancer is essential for providing stable and specific nucleation points for the formation of the polyaniline nanofibrous network. The acidity and mechanical agitation conditions are carefully adjusted to control the fibrous polyaniline. The embedded gallium elements form an initial seeding layer around the liquid metal nanoparticles. The novel nanocomposites offer synergistic properties for environmental sensing and molecular separation applications. This study provides a road map for the direct synthesis of long organic molecular chains at the dynamic interfaces of liquid metals.

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