Herein, a facile method for constructing acid‐base and CrIII species multi‐functionalized multi‐walled carbon nanotubes (CNTs) catalyst was reported. Acid and base, i.e., −SO3H and −NH2 groups, were first grafted on CNTs to synthesize CNTs−SO3H−NH2 bi‐functional catalyst. Then the obtained CNTs−SO3H−NH2 catalyst was further functionalized with CrIII species for further enhancement of acidity. The catalytic activity of fabricated catalysts were systematically studied for the one‐pot conversion of cellulose to 5‐hydroxymethylfurfural (HMF) in an ionic liquid solvent system. Results indicated that in the one‐pot cellulose to HMF reaction, acidic sites were necessary for dissolved cellulose hydrolysis and fructose dehydration process, and the isomerization of glucose to fructose can be regarded as rate determining step. Co‐existed base and Lewis acid sites were found to promote glucose isomerization to fructose, and Brønsted acid sites direct the dehydration of reactively formed fructose to HMF. And under the optimal conditions, the highest HMF yield of 40.2 % was achieved by multi‐functional CNTs−SO3H−NH2−CrIII catalyst. Moreover, the fabricated catalyst in this study revealed excellent stability for recycle use in HMF production from cellulose.