The application of renewable nanomaterials, like nanocrystalline cellulose (NCC), has recently been widely studied by many researchers. NCC has many benefits such as high aspect ratio, biodegradability, and high number of hydroxyl groups which offer great opportunities for modification. In this study, the NCC derived from empty fruit bunches (EFB) was modified with aminosilane, 3-(2-aminoethylamino)propyl-dimethoxymethylsilane (AEAPDMS), and the characterization was performed to investigate the potential as carbon dioxide (CO2) capture. Modification of NCC with AEAPDMS was carried out in water/ethanol solvent (80/20) (v/v) with a ratio of NCC to aminosilane of 1 : 1, 1 : 2, 1 : 3, and 1 : 4 w/w%. The effects of AEAPDMS on NCC were characterized using Fourier transform infrared (FTIR) spectroscopy, thermogravimetric analysis (TGA), X-ray diffraction (XRD) analysis, elemental analysis (CHNS), and transmission electron microscopy (TEM). The existence of AEAPDMS onto NCC was confirmed by ATR-FTIR spectroscopy as the new peaks of NH2were bending and wagging, and Si-CH3appeared. The thermal stability of NCC increased after modification due to the interaction with AEAPDMS. The elemental analysis result showed that the nitrogen content increased with an enhancement ratio of the modifiers. The XRD indicated that the crystallinity decreased while the rod-like geometry of NCC was maintained after amorphous AEAPDMS grafted on the NCC. Since AEAPDMS can be grafted on the NCC, the sample is applicable as CO2capture.