Studies on the influence of drying processes on cellulose nanofiber (CNF) aerogel performance has always been a great challenge. In this study, CNF aerogels were prepared via two different drying techniques. The CNF solution was prepared via existing chemical methods, and the resultant aerogel was fabricated through supercritical CO drying and liquid nitrogen freeze-drying techniques. The microstructure, shrinkage, specific surface area, pore volume, density, compression strength, and isothermal desorption curves of CNF aerogel were characterized. The aerogel obtained from the liquid nitrogen freeze-drying method showed a relatively higher shrinkage, higher compression strength, lower specific surface area, higher pore volume, and higher density. The N adsorption capacity and pore diameter of the aerogel obtained via the liquid nitrogen freeze-drying method were lower than the aerogel that underwent supercritical CO drying. However, the structures of CNF aerogels obtained from these two drying methods were extremely similar.