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Materials with negative Poisson's ratio have attracted considerable attention and offered high potential applications as biomedical devices due to their ability to expand in every direction when stretched. Although negative Poisson's ratio has been obtained in various base materials such as metals and polymers, there are very limited works on hydrogels due to their intrinsic brittleness. Herein, we report the use of methacrylated cellulose nanocrystals (CNCMAs) as a macro‐cross‐linking agent in poly(2‐hydroxyethyl methacrylate) (pHEMA) hydrogels for 3D printing of auxetic structures. Our developed CNCMA‐pHEMA hydrogels exhibit significant improvements in mechanical properties, which is attributed to the coexistence of multiple chemical and physical interactions between the pHEMA and CNCMAs. Structures printed by using CNCMA‐pHEMA hydrogels show auxetic behavior with greatly enhanced toughness and stretchability compared to the hydrogel with a traditional cross‐linking agent. Such strong and tough auxetic hydrogels would contribute toward establishing advanced flexible implantable devices such as biodegradable oesophageal self‐expandable stents. [ABSTRACT FROM AUTHOR]