Self‐Driving Laboratory Optimizes the Lower Critical Solution Temperature of Thermoresponsive Polymers

To overcome the inherent inefficiencies of traditional trial‐and‐error materials discovery, the scientific community is increasingly developing autonomous laboratories that integrate data‐driven decision‐making into closed‐loop experimental workflows. In this work, we realize this concept for thermoresponsive polymers by developing a low‐cost, ”frugal twin” platform for the optimization of the lower critical solution temperature (LCST) of poly(N‐isopropylacrylamide) (PNIPAM). Our system integrates robotic fluid‐handling, on‐line sensors, and Bayesian optimization (BO) that navigates the multicomponent salt solution spaces to achieve user‐specified LCST targets. The platform demonstrates convergence to target properties within a minimal number of experiments. It strategically explores the parameter space, learns from informative ”off‐target” results, and self‐corrects to achieve the final targets. By providing an accessible and adaptable blueprint, this work lowers the barrier to entry for autonomous experimentation and accelerates the design and discovery of functional polymers.