The feasibility of using raw diatomite and aluminum hydroxide-modified diatomite (Al-diatomite) for removal of aniline and phenol from water was investigated. Their physicochemical characteristics such as pHsolution, point of zero charge (pHPZC), surface area, Fourier transform infrared (FT-IR) and scanning electron microscopy was determined. After the raw diatomite was modified, the surface area of Al-diatomite increases from 26.67 to 82.65 m2 g–1. The pHPZC and pHsolution (10%) occurred around pH 5.2 and pH 8.6, respectively. The removal rates of aniline and phenol on diatomite and Al-diatomite decreased with increasing solution pH, while surface charge density decreased. The adsorption of aniline and phenol on diatomite presented a good fit to the Langmuir and Freundlich models, but the models are not fit to forecast the adsorption of aniline and phenol on Al-diatomite. The study indicated that electrostatic interaction was a dominating mechanism of aniline and phenol sorption onto Al-diatomite.