Provided herein are graphene nanoribbons with high structural uniformity and low levels of impurities and methods of synthesis thereof. Also provided herein are graphene nanoplatelets of superior structural uniformity and low levels of impurities and methods of synthesis thereof. Further provided herein are mixtures of graphene nanoribbons and graphene nanoplatelets of good structural uniformity and low levels of impurities and methods of synthesis thereof. The method includes, for example, the steps of depositing catalyst on a constantly moving substrate, forming carbon nanotubes on the substrate, separating carbon nanotubes from the substrate, collecting the carbon nanotubes from the surface where the substrate moves continuously and sequentially through the depositing, forming, separating and collecting steps. Further processing steps convert the synthesized carbon nanotubes to graphene nanoribbons, graphene nanoplatelets and mixtures thereof.