Cellulose detectors, as green sensors, are some of the defensive mechanisms of plants which combat environmental stresses. However, extracted cellulose struggles to fulfil these functionalities due to its rigid physical/chemical properties. In this study, a novel cellulose dual-crosslinked framework (CDCF) is proposed. This comprises a denser temporary physical crosslinking bond (hydrogen bonding) and a looser covalent crosslinking bond (N,N-methylenebisacrylamide), which create deformable spaces between the two crosslinking sites. Abundant pH-sensitive carboxyl groups and ultralight, highly porous structures make CDCF response very sensitive in acid/alkaline vapor environments. Hence, a significant shrinkage of CDCF was observed following exposure to vapors. Moreover, a curcumin-incorporated CDCF exhibited dual shape and color changes when exposed to acid/alkaline vapors, demonstrating great potential for the multi-detection of acid/alkaline vapors.