A series of amphiphilic double-brush polymers based on itaconate diesters were synthesized with the objective of tailoring the thermal and mechanical properties of hydrogels formed by them; the amphiphilic itaconate diesters carried an MPEG350 segment and an alkyl chain, whose length was varied from C12 to C18. As was reported by us earlier ( 50, 5004), the formation of the hydrogel was due to the crystallization of alkyl segments, as confirmed by the match of the rheological gel-to-sol transition with that of differential scanning calorimetry melting transition of the gel. In an effort to fine-tune the hydrogel-melting temperature and its strength, we varied the length of the alkyl chain length while keeping the hydrophilic segment length constant at MPEG350; apart from varying the alkyl chain length, an oxyethylene spacer was incorporated to examine the effect of decoupling the alkyl side-chain crystallization from the backbone. With these modifications, the melting temperature of the hydrogel was varied from 30 to 56 °C. Likewise, the strength of the hydrogel, as reflected by its storage modulus, varied from around 220 to 970 Pa; the softer gels typically exhibited a slightly larger critical shear strain beyond which the gel transformed into a sol. The thermal and shear-induced gel-to-sol transitions were reversible; however, the modulus after the shear-induced transition did not fully recover instantly (∼80%), suggesting that the formation of the extended gel network is slow. Further fine-tuning could be achieved by copolymerization of two different amphiphilic itaconate monomers, namely, those with C16 and C18, which provided an intermediate gel-melting temperature; however, co-gelation of the two preformed homopolymer gels yielded two distinct gel-melting transitions. Thus, this class of tuneable stimuli-responsive polymeric hydrogels prepared from biobenign components, namely, itaconic acid, 1-alkanols, and MPEGs, could serve as potential candidates for biomedical applications.