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The combination of thermoresponsive polymers and biopolymers is growing due to the multiple beneﬁts, owing to their tunable properties. Numerous works focus on the preparation of materials by chemical cross-linking, but physical cross-linking (based on hydrogen bonding) has not been deeply studied. In this context, questions around the hydrogen bonding of physical-crosslinking and lower critical solution temperature (LCST) need to be addressed, especially when a second comonomer is incorporated. This study is based on the preparation of blends of poly(N-isopropylacrylamide-co-N-ethylacrylamide) copolymers and carboxymethyl cellulose (CMC) by dis-solution, where the LCST-transition and physical-crosslinking are studied. The results show a strong eect of the comonomer on the properties in compar-ison with the CMC, especially for solutions of methanol/water. Low contents of N-ethylacrylamide (NEAM) can promote physical-crosslinking and the gela-tion, avoiding cononsolvency observed for homopolymers. On the other hand, NEAM will disrupt the gelation when the comonomer content is high enough.