Graft copolymers based on a poly(dehydroalanine) (PDha) backbone and different hydrophilic or hydrophobic side chains were synthesized. Graft copolymers containing a diethyl glycidyl amine side chain displayed lower critical solution temperature (LCST)-type thermo-responsive behaviour and were applied to prepare thermo-responsive hydrogels. Amphiphilic graft copolymers containing aliphatic or aromatic side chains were able to encapsulate a wide variety of fragrances. The robustness of these graft copolymers towards many different fragrances and combinations of different side chains proves the applicability of PDha-based graft copolymers for all sorts of encapsulation systems.