Graphene is a two-dimensional carbon structure that exhibits remarkable structure-property relations. Consequently, there has been immense effort undertaken towards developing methods for graphene synthesis. Chemical vapor deposition (CVD) and chemical exfoliation from colloidal suspensions are two common methods used for obtaining graphene films. However, the underlying experimental conditions have to be carefully optimized in order to obtain graphene films of controllable thickness and morphology. In this context, a significant part of this dissertation was devoted towards developing and improving current CVD-based and chemical exfoliation based methods for synthesizing high quality graphene films. Specifically, in the CVD based procedure for growing graphene on copper, the effect of surface pretreatment of copper was investigated and the quality of graphene grown using two different pretreatment procedures was compared and analyzed. In particular, graphene grown on electropolished copper (EP-Cu) was analyzed with respect to its surface morphology, surface roughness and thickness, and compared with graphene grown on as cold-rolled acetic acid cleaned copper (AA-Cu). It was shown that electropolishing of the Cu substrates prior to graphene growth greatly enhanced the ability to obtain flat, uniform, predominantly single layer graphene surface coverage on copper. The reported surface roughness of the graphene on EP-Cu was found to be much lower than for previously reported systems, suggesting that the electropolishing procedure adopted in this work has great promise as a pretreatment step for Cu substrates used in CVD growth of graphene. Obtaining graphene from colloidal suspensions of graphitic systems was also examined. In this work, an acid (H₂SO₄ + HNO₃) treatment process for intercalating natural graphite flakes was examined and the ability to reversibly intercalate and deintercalate acid ions within graphitic galleries was investigated. More importantly, a rapid-thermal expansion (RTP) processing was developed to thermally expand the acid-treated graphite, followed by exfoliation of predominantly bilayer graphene as well as few layer graphene flakes in an organic solvent (N, N-Dimethylformamide - DMF). The developed method was shown to provide bilayer and few layer graphene flakes in a reliable fashion. Fullerene is another carbon nanostructure that has garnered attention due to unique structure and chemical properties. Recently, there has been increased focus towards harnessing the properties of fullerenes by synthesizing fullerene self-assemblies in the form of extended rods, tubes and more complex shapes. Current methods to synthesize these self-assemblies are either cumbersome, time consuming or expensive. In this context, an alternate, straightforward dip-coating procedure technique to self-assemble equal-sized, faceted, polymerized fullerene nanorods on graphene-based substrates in a rapid fashion was developed. By suitably modifying the kinetics of self-assembly, the ability to reliably control the spatial distribution, size, shape, morphology and chemistry of fullerene nanorods was achieved.