Polythiophene/graphene oxide (PTh/GO) nanocomposite (NC) was prepared through polymerisation of thiophene in the presence of GO and was used for mercury ions (Hg2+) adsorption in aqueous solutions. Equilibrium studies showed that mercury removal was strongly influenced by solution pH and GO composition in the NC. The equilibrium data were well described by both Langmuir and Freundlich isotherm models, with a Langmuir maximum adsorption capacity of 113.6 mg/g. Adsorption kinetics were rapid and correlated well with the pseudo-second-order model. The thermodynamic studies indicated that the adsorption was spontaneous and endothermic in nature, and occurred through a physicochemical mechanism. Desorption studies revealed that PTh/GO NC could be used repeatedly for three adsorption-desorption cycles without a significant loss in its capacity. Competing ions reduced mercury uptake although considerable values were still attained. The findings of this study suggest that PTh/GO NC is a potential adsorbent for Hg2+ removal from aqueous solutions.