In this work, we took advantage of the versatility of polymer chemistry for developing a tuneable, temperature-responsive, peptide-crosslinked polymeric nanogel platform for enzyme-triggered biomolecule delivery. Via copolymerisation of NIPAM with NCPAM we could tune the thermal behaviour of the resulting copolymers resulting in a range of Tcp values around body temperature (from 33 to 44 °C). A peptide-based cross-linking approach was developed to covalently constrain the nanogel-forming copolymer chains to increase stability and equip the nanocarrier platform with enzyme-responsiveness. We obtained high-quality morphological information on the self-assembled structures, successfully studied dynamic behaviours upon temperature changes and cross-linking, as well as model protein loading and enzyme-triggered release by employing a combination of cryo-TEM, SANS and FCS. This detailed analysis yielded a morphology of filled spheres (imaged with cryo-TEM) that relaxed to an interconnected polymer network upon cross-linking and lowering the temperature below the LCST as found by SANS measurements. Even further, the coil-to-globule transition of one selected copolymer was successfully monitored in real-time by SANS. Model enzymetriggered (MMP-7) particle disassembly and accompanying increase in cargo release kinetics was determined by employing FCS. Our modular platform features the following key characteristics: reproducible, simple and fast temperature-induced nanogel assembly, modulation of the self-assembly temperature via copolymerisation of NIPAM and NCPAM in the thermo-sensitive block, containing two distinct handles (carboxylic groups and alkynes)