We designed triblock copolymers to confer the final self-assembled nanogels with favourable properties for enzyme-triggered drug delivery applications (Scheme 1). Conceptually, an inert hydrophilic block (Scheme 1, dark blue), which we expected to form the corona of the assembled nanogels, was connected to a thermo-sensitive block (Scheme 1, light blue/green) which would drive self-assembly at temperatures above its LCST. We chose to use PEG as the hydrophilic block and either PNIPAM, PNCPAM or copolymers of the two P(NIPAM-co-NCPAM) as the thermo-responsive block. Between these two blocks we incorporated a functional block (Scheme 1, red) composed of a mixture of methacrylic acid (MAA) and trimethylsilylpropargylmethacrylate (TMSPMA) to provide a latent handle for cross-linking with azide-bi-functionalised peptide after self-assembly and desilylation. We used RAFT polymerisation for the synthesis of these polymers, due to the ease of preparing well-defined multi-block copolymers and PNIPAM via this route. The detailed synthetic procedure is shown in Scheme 2.