New application of modified silica aerogel nanoparticles was carried out for adsorption of Vietnamese spilled crude oil obtained from Bach-Ho field. The aerogel was synthesized by atmospheric drying method without critical extraction procedure in liquefied CO2 followed by surface modification using polydimethylsiloxane precursor in n-hexane solvent. The synthesis mixture contained precise amounts of water, tetraethyl orthosilicate (TEOS), ethanol and HCl with volume ratios of 2:1:4:0.0003, respectively. The modification was established by the mixing of the as-synthesized aerogel and polydimethylsiloxane followed by calcination at 350 ºC for 4 h obtaining the surface modified aerogel. The modified aerogel was applied in the adsorption of the spilled crude oil in mild temperature and atmospheric pressure. Some techniques such as X-ray diffraction (XRD), transmission electron microscopy (TEM), Brunauer-Emmett-Teller surface area analysis (BET) and Fourier transform infrared spectroscopy (FTIR) were used for characterizing the materials.