A freeze-thaw technique is put forth as a novel approach to exfoliating graphene oxide sheets (GO-sheets) in aqueous media. This method does not use shear force or high-temperature treatment at any stage. Avoiding these factors prevents scrolling and promotes defect-free synthesis of the graphitic planes. The research shows how the freeze-thaw technique successfully exfoliates graphitic planes without producing scrolls or defective graphene oxide planes. Further, when compared to conventional exfoliation methods, it was found that the freeze-thaw technique increased the surface area significantly.