Two-dimensional nanomaterials have been incorporated into coating layers for exceptional properties in mechanic toughness, electronics, thermology and optics. Graphene oxide (GO), however, was greatly hindered by its strong adsorption within visible wavelength and hereby the intrinsic dark color at the solid state. Herein, we found a unique aqueous mixture of GO containing sodium dodecyl sulfate and l-ascorbic acid. It enabled to produce iridescent coating layers with tunable thickness of 0.3–50 μm on both hydrophilic and hydrophobic substrates (e.g., glass, aluminum foil, polytetrafluoroethylene), through brushing, liquid-casting, dipping and writing. Their iridescence could be further tuned by incorporating MXene nanosheets. And their mechanical properties could be enhanced by certain synthetic polymers (e.g., polyvinyl alcohol and polyethylene glycol). Their sensitivity to heat, laser and water also benefited to pattern the coating layers. Furthermore, by controlling laser intensity, the domain color could be changed (e.g., green to blue). Thus, this study may pave a new pathway of producing iridescent coatings of graphene oxide in a large scale for practical applications.