Thermosensitive polymers show an entropy-driven transition from a well-solvated to a poorly solvated polymer chain, resulting in a more compact globular conformation. The transition at the lower critical solution temperature (LCST) is often sharp, which allows for a wide range of smart material applications. At the LCST, oligo(ethylene glycol)-substituted polyisocyanides (PICs) form soft hydrogels, composed of polymer bundles similar to biological gels, such as actin, fibrin and intermediate filaments. Here, we show that the LCST of PICs strongly depends linearly on the length of the ethylene glycol (EG) tails; every EG group increases the LCST and thus the gelation temperature by nearly 30 °C. Using a copolymerisation approach, we demonstrate that we can precisely tailor the gelation temperature between 10 °C and 60 °C and, consequently, tune the mechanical properties of the PIC gels.