Cobalt ferrite nanoparticles (CFO NPs) are synthesized by a facile and polyethylene glycol (PEG) assisted hydrothermal method. In the synthesis of cobalt ferrites, PEG is used as a surfactant. The formation of single-phase spinel structure in the samples is confirmed by XRD patterns. TEM images show that the addition of PEG results in the decrease in the size of the CFO NPs. When the amount of PEG is lower than 2.4 g, the particle sizes decrease, then, further increasing the concentration of PEG in the solution, the particle sizes begin to increase, for much more PEG will cover onto the surface of the nanoparticles. Here, the existence of PEG on the surface of CFO NPs is confirmed from the characteristic bands of PEG in FTIR spectra. All the samples are ferromagnetic, and their saturation magnetization (Me) decreases with the increase in PEG concentration. The as-synthesized samples show highly selective adsorption characteristics for organic dyes. Compared with methyl orange (MO) and methyl blue (MB) dyes, good adsorption performance of the PEG/CoFe2O4 nanocomposites for Congo red (CR) dye is presented. Moreover, the addition of PEG greatly enhances their adsorption capacity (q(e)) for CR. The corresponding adsorption behavior fits well with the pseudo-second-order kinetic model and the Langmuir model. And the adsorption mechanism is investigated. This study suggests that the as-prepared products can be regarded as an excellent selective adsorbent to remove dyes from the wastewater. (C) 2016 Elsevier B.V. All rights reserved.