Biomass aerogels have received extensive attention due to their unique natural characteristics. However, biomass-based chitosan aerogels are often confronted with the traditional issue concerning a weak skeleton structure, namely, the corresponding huge shrinkage for chitosan aerogels in the stage from the final gel to the aerogel. Herein, we put forward a new approach to enhance chitosan aerogels by introducing natural biomaterial cellulose nanocrystal (CNC). CNC is applied to connect/cross-link chitosan chains to form its networking construction through supramolecular interaction/physical entanglement, eventually realizing the enhancement of the chitosan aerogel network structure. Chitosan aerogels modified with CNC exhibit a high specific surface area of 578.43 cm2 g-1, and the pore size distribution is in the range of 20-60 nm, which is smaller than the mean free path of gas molecules (69 nm), triggering a "no convection" effect. Hence, the gaseous heat transfer of chitosan aerogel is effectively suppressed. Chitosan aerogels with the addition of CNC show an excellent thermal insulation property (0.0272 W m-1 K-1 at ambient condition) and an enhanced compressive strength (0.13 MPa at a strain of 3%). This improvement method of chitosan aerogel in enhancing the skeleton structure aspect provides a new kind of idea for strengthening the nanoscale morphology structure of biomass aerogels.