Carbon nanotubes and graphene offer great promise but also face significant challenges for future beyond-silicon nanoelectronics. This talk will focus on our recent work on nanoelectronics based on aligned nanotubes, macroelectronics based on separated nanotubes, and wafer-scale CVD graphene. We have developed the synthesis of massively aligned single-walled carbon nanotubes atop sapphire and quartz substrates, and we will also present our recent progress toward type-controlled and chirality-controlled carbon nanotube synthesis. In addition, we will report macroelectronics based on separated nanotube thin film transistors, including key technology components such as assembly of separated nanotube networks, high-yield fabrication of devices, and applications for AMOLED displays and printed electronics. Furthermore, we will present scalable fabrication of self-aligned T-gate graphene transistors for RF applications.