We developed a surface-chemistry-based approach to investigating the influence of surface functionalization on the growth of gold nanostructures on graphene thin films by utilizing various pyrene derivatives presenting different functional groups. Among the surface-modifying molecules, decylpyrene (DP) yielded the highest content of gold rods (average 22 +/- 4%) among gold nanostructures on graphene films when a graphene surface was pretreated with DP prior to gold nanostructure growth. The improved yield of gold rods on graphene thin films enhanced several physical properties of graphene such as the electrical conductivity and Raman signals by 6.3- and 14.7-fold, respectively.