Technologies are presented for growing graphene by chemical vapor deposition (CVD) on a high purity copper surface. The surface may be prepared by deposition of a high purity copper layer on a lower purity copper substrate using deposition processes such as sputtering, evaporation, electroplating, or CVD. The deposition of the high purity copper layer may be followed by a thermal treatment to facilitate grain growth. Use of the high purity copper layer in combination with the lower purity copper substrate may provide thermal expansion matching, compatibility with copper etch removal, or reduction of contamination, producing fewer graphene defects compared to direct deposition on a lower purity substrate at substantially less expense than deposition approaches using a high purity copper foil substrate.