Engineering the Charge Transport of Ag Nanocrystals for Highly Accurate, Wearable Temperature Sensors through All‐Solution Processes

All‐nanocrystal (NC)‐based and all‐solution‐processed wearable resistance temperature detectors (RTDs) are introduced. The charge transport mechanisms of Ag NC thin films are engineered through various ligand treatments to design high performance RTDs. Highly conductive Ag NC thin films exhibiting metallic transport behavior with high positive temperature coefficients of resistance (TCRs) are achieved through tetrabutylammonium bromide treatment. Ag NC thin films showing hopping transport with high negative TCRs are created through organic ligand treatment. All‐solution‐based, one‐step photolithography techniques that integrate two distinct opposite‐sign TCR Ag NC thin films into an ultrathin single device are developed to decouple the mechanical effects such as human motion. The unconventional materials design and strategy enables highly accurate, sensitive, wearable and motion‐free RTDs, demonstrated by experiments on moving or curved objects such as human skin, and simulation results based on charge transport analysis. This strategy provides a low cost and simple method to design wearable multifunctional sensors with high sensitivity which could be utilized in various fields such as biointegrated sensors or electronic skin. All‐solution processed and all‐nanocrystal (NC)‐based wearable temperature sensors are fabricated. Silver NC layers with both positive and negative temperature coefficients of resistance are achieved by engineering the charge transport mechanism through ligand exchange. One‐step photolithography methods are developed to design motion‐free sensors by integrating two NC layers into one ultrathin device.