Kaolinite-supported nanoscale zero-valent iron (K-nZVI) was successfully synthesized as a multifunctional composite and used for the degradation of crystal violet (CV). The presence of kaolinite not only decreased the aggregation of zero-valent iron nanoparticles (nZVI) with maintenance of reactivity, but also facilitated reaction by increasing the local concentration of CV in the vicinity of nZVI as an adsorbent. This was confirmed by scanning electron microscopy (SEM) and batch experiments, which showed that 97.23% of CV was removed using K-nZVI, while only 78.72% and 39.22% of CV were removed using nZVI and kaolinite after 30 min, respectively. Different factors impacting on degradation of CV were investigated as well. On the basis of these results, a removal mechanism was proposed including: (i) prompt adsorption of CV to the K-nZVI phase, and (ii) reduction of CV by Fe-0 on K-nZVI. Furthermore, different adsorption and reduction kinetics were employed to examine the removal process of CV, where a better fit with the pseudo-second-order model for adsorption and pseudo-first-order model for reduction process was observed, and reduction was the rate limiting step. In addition, isotherm and thermodynamic parameters were evaluated for a specific study of the important adsorption step. Finally, the application of K-nZVI to treat wastewater showed the removal efficiency higher than 99.9%. (C) 2013 Elsevier Inc. All rights reserved.