The aim of this project is to understand and control the fundamental physical properties of novel carbon nanomaterials:carbon nanotubes and graphene. By a combination of complementary methods, i.e. vibrational spectroscopy, scanning probe microscopy, and theoretical modelling, a comprehensive understanding of the electronic, vibrational, optical properties, and their connection with the material’s structure will be obtained. A diagnostics “toolbox” will be established on the materials intheir most unperturbed, ideal states. Taking the results as reference, the materials will be studied under conditions relevant when incorporated into devices. These include imperfections of the materials and interaction with different environments, with other carbon nanotubes/graphene, and with extrinsic materials introduced during device processing. The gained insight and understanding on a fundamental level will also advance technological routes for scaling up carbon-nanomaterial electronic device fabrication, which is still lacking sufficient control over selectivity towards the desired physical properties. Control over the electronic and optical properties will be sought through deliberately induced interactions and chemical functionalizationof the materials. The project benefits from close collaborations between experimental and theoretical physics, chemistry, and materials science.