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This chapter focuses on thermally responsive polymers and their building blocks. Starting from polymeric assemblies in solutions, going into solids with stimuli-responsive transitions, a comprehensive summary of existing monomers capable of thermal responses is provided. The attractiveness of temperature-responsive homo- and copolymers is primarily driven by the ability of macromolecular segments to undergo conformational changes at a designated temperature. The earliest reports of the thermal phase transitions in poly(N-isopropylacrylamide) (PNIPAM) go back to the late 1960s, and this still continues to be an important and advantageous area in controlled drug delivery, bioseparation, enzyme activity, filtration, and mediating surface/interfacial properties. The last section of this chapter focuses in the thermally responsive peptides, their stimuli-responsiveness, selected applications, and examining the general principles governing the role of entropic contributions to stimuli-responsiveness.

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