A widely soluble graphene sheet/Congo red (GSCR) composite was synthesized and applied to prepare GSCR/Au hybrid materials. UV-vis absorption, Fourier transform infrared, Raman, and X-ray photoelectron spectra revealed that Congo red (CR) is successfully coupled on graphene sheets. The morphology of GSCR was studied by transmission electron microscopy, scanning electron microscopy, and atomic force microscopy. The dispersion behavior of the GSCR composite was also studied in 18 different solvents, and the digital images indicate that it is soluble both in water and in a variety of organic solvents. The GSCR nanosheets are still single layers or bilayers in water and individual from one to another after 100 days of storage. Furthermore, the mechanism of GSCR's good solubility was successfully explained by the Hansen solubility parameters. The four standard probe result shows that the GSCR films have a bulk conductivity of approximately 6850 S m(-1). The wide solubility and long lifetime of GSCR solutions are absolutely necessary for further treatment. As an example, Au nanoparticles densely decorated CR-functionalized graphene sheets through electrostatic interaction.