Graphene oxide (GO) was cross-linked with chitosan to yield a composite (GO-LCTS) with variable morphology, enhanced surface area, and notably high methylene blue (MB) adsorption capacity. The materials were structurally characterized using thermogravimetric analysis and spectroscopic methods (X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, and 13 C solid-state NMR) to support that cross-linking occurs between the amine groups of chitosan and the −COOH groups of GO. Equilibrium swelling studies provide support for the enhanced structural stability of GO-cross-linked materials over the synthetic precursors. Scanning electron microscopy studies reveal the enhanced surface area and variable morphology of the cross-linked GO materials, along with equilibrium and kinetic uptake results with MB dye in aqueous media, revealing greater uptake of GO-LCTS composites over pristine GO. The monolayer uptake capacity ( Q m ; mg g –1 ) with MB reveals twofold variation for Q m , where GO-LCTS (402.6 mg g –1 ) > GO (286.9 mg g –1 ). The kinetic uptake profiles of MB follow a pseudo-second-order trend, where the GO composite shows more rapid uptake over GO. This study reveals that the sorption properties of GO are markedly improved upon formation of a GO–chitosan composite. The facile cross-linking strategy of GO reveals that its physicochemical properties are tunable and versatile for a wider field of application for contaminant removal, especially over multiple adsorption–desorption cycles when compared against pristine GO in its highly dispersed nanoparticle form.

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