Recently there has been interest in two-dimensional graphene-based superstructures, such
as twisted bilayer or trilayer graphene or graphene on hexagonal boron nitride, stacked one
on top of the other. These superstructures are expected to have electronic and optical properties
that depend on even small changes in the twist angles. By structural mapping in the
micrometer scale, we demonstrate that superstructures consist of stacking-induced ‘superlattice
domains’. The rotational disorder between domains created by the superstructural
defects, such as wrinkles, folds and grain boundaries, and guest species intercalated
between stacked layers, was analyzed at a resolution of sub-one degree. This comprehensive
approach provides crucial structural information on graphene-based superstructures.