Carbon-based materials, like the one-dimensional carbon nanotubes (CNT) and the two-dimensional graphene, attract a lot of interest for the development of novel nanoelectronic devices, owing to their particular properties such as superior carrier mobility. The increased miniaturization of these carbon-based devices offers, however, new challenges. First, because of the devices’ very small dimensions in one or more directions, (sometimes unforeseen) quantum effects come into play. Simulation tools to support the design of these new quantum devices need to model the complex quantum mechanical behavior of the charge carriers whilst also still taking all electromagnetic phenomena into account. Second, the unavoidable manufacturing tolerances entail another modeling challenge, as they introduce variability in the miniaturized devices’ geometrical parameters and materials characteristics. This variability affects the devices’ performance and, thus, it needs to be quantified and considered during design. The overall goal of the proposed project is to develop uncertainty quantification (UQ) tools which can be employed during the design of novel carbon-based nanodevices. Specifically, leveraging generalized polynomial chaos expansions, non-intrusive and intrusive UQ schemes for Maxwell/Schrödinger and Maxwell/Dirac systems, describing CNT-based and graphene-based nanodevices respectively, will be developed and implemented.