Thermal, mechanical, and surface properties of a library of poly(2‐oxazoline)s are investigated. These polymers are suitable to study structure/property relationships as their cationic ROP and the relative facile monomer synthesis allow for control over the molecular structure. The number of carbon atoms in the linear side‐chain is systematically varied from methyl to nonyl. Relations between chemical structures, thermal transitions, surface energies, and elastic moduli are discussed. It is shown that the mechanical and thermal properties of the polymers depend on the presence of a crystalline phase in the material. The amorphous polymers reveal a decrease in the reduced moduli along with a decrease in their respective glass transition temperature with increasing length of the side‐chain.
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