Graphene oxide (GO) was synthesized and employed as an adsorbent for Zn(II) removal from an aqueous solution. The adsorption isotherms showed that Zn(II) adsorption can be better described using the Freundlich model than the Langmuir model. The maximum adsorption capacity of Zn(II) on GO determined using the Langmuir model at pH 7.0 and 293 K was 208.33 mg/g. The calculation of thermodynamic parameters revealed that the process of Zn(II) adsorption on GO was chemisorptions, endothermic, and spontaneous. Kinetic studies indicated that the pseudo-second-order kinetic model showed a better simulation of Zn(II) adsorption than the pseudo-first-order kinetic model. On the basis of surface complexation modeling, the double layer model provided a satisfactory prediction of Zn(II) by inner-sphere surface complexes (for example, SOZn+ and SOZnOH species), indicating that the interaction mechanism between Zn(II) and GO was mainly inner-sphere complexation. In terms of reusability, GO could maintain 92.23% of its initial capability after six cycles. These findings indicated that GO was a promising candidate for the immobilization and preconcentration of Zn(II) from aqueous solutions.