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A highly effective flame retardant (FR) nanocoating was developed by conducting oxidative polymerization of dopamine monomer within an aqueous liquid crystalline (LC) graphene oxide (GO) scaffold coating. Due to its high water content, the LC scaffold coating approach facilitated fast transport and polymerization of dopamine precursors into polydopamine (PDA) within the water swollen interlayer galleries. Uniform and periodically stacked (14.5 Å d‐spacing) PDA/GO nanocoatings could be universally applied on different surfaces, including macroporous flexible polyurethane (PU) foam and flat substrates such as silicon wafers. Remarkably, PDA/GO coated PU foam exhibited highly efficient flame retardant performance reflected by a 65% reduction in peak heat release rate at 5 wt% PDA/GO loading in an 80 nm thick coating. While many physically mixed flame retardants are usually detrimental to the …