Hydrogels based on hydrophobic, or micellar interactions, are physically crosslinked hydrogels which are an attempt to overcome the poor mechanical properties of traditional, chemically crosslinked gels, such as low shear strength. We have prepared a polysaccharide‐based hydrogel with physical crosslinks via hydrophobic interactions. In this work, we have synthesized hydrogel by grafting a hydrophobic moiety dioctylamine onto hydrophilic precursor carboxymethyl cellulose (CMC) through an amide bond formation, where ~33% of the carboxyl group in CMC was reacted with dioctylamine. The thermosensitive hydrogel can arrest 100 mL of deionized water per gram of gelator within few seconds. It showed the moderate rheological property. The hydrogel is nontoxic and does not show any adverse to human hemoglobin. It is a CMC based a unique gelator with high biocompatibility represent to be useful materials for biomedical application. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47665.