Nanocellulose, owing to its environmentally friendly and unique attributes, is gaining traction in various industries. However, commercialization of nanocellulose faces challenges due to structural alterations during drying process, leading to irreversible aggregation. This study, inspired by wood’s natural structure, introduces a cellulose nanofibril (CNF) drying system using hemicellulose hydrolysate (HH) as a capping agent. The addition of only 1 wt% of HH to the CNF suspension not only prevents aggregation among CNFs during dehydration and drying but also dramatically enhances the redispersion rate and dispersion stability of the dried CNFs. The redispersed CNF/HH suspension exhibits physicochemical properties comparable to the original CNF suspension before drying. This confirms that HH inhibits irreversible hydrogen bonding among CNFs, leading to the restoration of the nanostructure during redispersion. Moreover, HH in the CNF suspension after redispersion can be easily removed through a simple water rinsing process, highlighting HH as a highly suitable candidate for preventing aggregation of CNFs.