Systems and methods for preparing films using sequential ion implantation, and films formed using same, are provided herein. A structure prepared using ion implantation may include a substrate; an embedded structure having pre-selected characteristics; and a film within or adjacent to the embedded structure and including ions having a perturbed arrangement arising from the presence of the embedded structure. The perturbed arrangement may include the ions being covalently bonded to each other, to the embedded structure, or to the substrate, whereas the ions instead may be free to diffuse through the substrate in the absence of the embedded structure. The embedded structure may inhibit or impede the ions from diffusing through the substrate, such that the ions instead covalently bond to each other, to the embedded structure, or to the substrate. The film may include, for example, diamond-like carbon, graphene, or SiC having a pre-selected phase.