Combining experiments and all-atom molecular dynamics simulations, we study the conformational behavior of polyacrylamide (PAM) in aqueous alcohol mixtures over a wide range of temperatures. This study shows that even when the microscopic interaction is dictated by hydrogen bonding, unlike its counterparts that present a lower critical solution temperature (LCST), PAM shows a counterintuitive tunable upper critical solution temperature (UCST)-type phase transition in water/alcohol mixtures that was not reported before. The phase transition temperature was found to be tunable between 4 and 60 °C by the type and concentration of alcohol in the mixture as well as by the solution concentration and molecular weight of the polymer. In addition, molecular dynamics simulations confirmed a UCST-like behaviour of the PAM in aqueous alcoholic solutions. Additionally, it was observed that the PAM is more swollen in pure alcohol solutions than in 80% alcoholic solutions due to θ-like behaviour. Additionally, in the globular state, the size of the aggregates was found to increase with increasing solvent hydrophobicity and polymer concentration of the solutions. Above its phase transition temperature, PAM might be present as individual polymer chains in the coil state (≤10 nm). As PAM is a widespread polymer in many biomedical applications (gel electrophoresis, etc.), this finding could be of high relevance for many more practical applications in high performance pharmaceuticals and/or sensors.