In this study, nanocrystalline cellulose (NCC) was used for reinforcement and formaldehyde (HCHO) adsorption of urea-formaldehyde (UF) resin adhesive in fiberboard. The original NCC was modified by 3-aminopropyltriethoxysilane for improving the wetting property with UF resin adhesive. The UF resin adhesive with modified NCC was analyzed by X-ray powder diffraction, thermogravimetric analysis, and Fourier transform infrared. The HCHO emission and bending and bonding strength of the UF resin adhesive with modified NCC were tested according to Chinese National Standard GB/T 17657-1999. Compared with the original UF resin adhesive, modified NCC led to limited effects on the crystal structure, thermal stability, and characteristic absorption peaks of UF resin adhesive. The HCHO emission of the UF resin adhesive with 1.0% modified NCC decreased by 13.0%, while the bending and bonding strength increased by 40.5 and 158.3%, respectively. The improvements of modified UF resin adhesive were destroyed by the reunion of NCC when the content was more than 1.5%.