Optical materials with colour-changing abilities have been explored for display devices1, smart windows2,3, or modulation of visual appearance4–6. The efficiency of these materials, however, has strong wavelength dependence, which limits their functionality to a narrow spectral range. Here, we report graphene-based electro-optical devices with unprecedented optical tunability covering the entire electromagnetic spectrum from the visible to microwave. We achieve this non-volatile and reversible tunability by electro-intercalation of lithium into graphene layers in an optically accessible device structure. This unique colour-changing capability, together with area-selective intercalation, inspires fabrication of new multispectral devices, including display devices and electro-optical camouflage coating. We anticipate that these results provide realistic approaches for programmable smart optical surfaces with a potential utility in many scientific and engineering fields.