AbstractCellulose-silica composite fiber samples have been successfully synthesized using cellulose solution, tetraethoxysilane, and NH3•H2O in ethanol/water mixed solvents at room temperature for 24 h. The cellulose solution was previously prepared by the dissolution of microcrystalline cellulose in a solvent mixture of N,N-dimethylacetamide (DMAc)/lithium chloride (LiCl). The effect of the tetraethoxysilane concentration on the product was investigated. The products were characterized by X-ray powder diffraction (XRD), thermogravimetric analysis (TG), differential scanning calorimetric analysis (DSC), scanning electron microscopy (SEM), Fourier transform infrared spectrometry (FT-IR), energy-dispersive X-ray spectrum (EDS), and cross polarization magic angle spinning (CP/MAS) solid state 13C-NMR. The morphology of the cellulose-silica composite fiber was investigated by SEM, while their composition was established from EDS measurements combined with the results of FT-IR spectral analysis and XRD patterns. The XRD, FT-IR and EDS results indicated that the obtained product was cellulose-silica composite fiber. The SEM micrographs showed that the silica particles were homogeneously dispersed in the cellulose fiber. The CP/MAS solid state 13C-NMR results indicated that the silica concentration had an influence on the crystallinity of the cellulose. This method is simple for preparation of cellulose-based composites.