In this work, a novel nanocomposite hydrogel based on cellulose nanocrystal (CNC) and chitosan (CS) was fabricated and applied as a carrier for the controlled delivery of theophylline. CNC was firstly periodate-oxidized to obtain dialdehyde nanocellulose (DACNC). Then, chitosan was crosslinked using DACNC as both the matrix and crosslinker in different weight ratios, to fabricate CNC/CS composites. The prepared composites were characterized using Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction pattern (XRD), scanning electron microscopy (SEM), zeta potential measurement and swelling ratio tests. FT-IR results confirmed the successful reaction between the free amino groups on chitosan and the aldehyde groups on DACNC. With the increase of chitosan percentage in the hydrogel, the isoelectric point was shifted towards an alkaline pH, which was probably caused by the higher content of free amino groups. The swelling ratio of the composite also increased, which may have been due to the decrease of crosslinking density. Because the swelling ratio of the drug-loaded hydrogels differed under varied pH values, the cumulative drug release percentage of the composite hydrogel was achieved to approximately 85% and 23% in the gastric (pH 1.5) and intestinal (pH 7.4) fluids, respectively. Therefore, CNC/CS hydrogel has application potential as a theophylline carrier.