In the present study, capability of nanodiamond (ND) for the adsorption of anionic (methyl orange, MO) and cationic (methylene blue, MB) dyes from aqueous solution was investigated. Employing fourier transform infrared (FTIR) spectroscopy, Boehm titration method and zeta potential, it was found that the simple thermal oxidation of ND at 425 degrees C, increased the content of carboxylic acid of ND and accordingly the zeta potential of ND decreased considerably. Therefore, a series of oxidized NDs (OND) at various oxidation times and as-received untreated ND (UND) was used as adsorbents of MO and MB. The adsorption experiments exhibited that UND had large adsorption capacity, very fast adsorption kinetics and excellent selectivity for MO over MB. These results suggested that the adsorption tendency of UND toward anionic MO dye followed not only by electrostatic interactions but also via the chemical interaction caused by the strong hydrogen bond between the sulfonate groups of MO and the oxygen containing groups on the surface of UND. In contrast, ONDs exhibited higher adsorption capacity for cationic MB whose tendency toward MB increased by increasing the thermal oxidation time due to the promotion of the negative charge on the surface of OND leading to the higher electrostatic attraction. The adsorption rate of MB on ONDs was also very high. Kinetics data was well fitted with the pseudo- second-order model for most of the adsorbents. The adsorption selectivity analysis revealed that ONDs displayed more adsorption capacity for MB compared with MO which was also attributed to high electrostatic interactions of cationic dye with negative charges of ONDs. Finally, the release behavior of NDs was also demonstrated after soaking in ethanol and acetone. (C) 2018 Elsevier Inc. All rights reserved.