This Dissertation presents work that furthers the understanding of polymer degradation under rapid thermal annealing (RTA) and how it is advantageously utilized for the doping and healing of graphene. Our newly established method of post-synthesis graphene doping/healing, dubbed the “nanobandage” method, applies a thin film of dopant-containing polymer that is degraded via RTA to drive dopants into the graphene. A model system of nitrogen-doping polyethylenimine (PEI) on monolayer graphene is employed for the initial study, and nitrogen doping in the graphene matrix is verified via Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and electrical testing, where graphene samples with a higher amount of defects exhibit greater doping levels. The degradation of PEI and subsequent incorporation into graphene defects is then explored via a tandem experimental and computational study. Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) and reactive molecular dynamics (RMD) simulations are employed to provide data of the entire degradation process to an extent that just one method alone cannot cover. Thirteen potential key fragments for doping are identified from Py-GC/MS, and combined with the knowledge from the RMD simulations, establish a pathway from degradation to doping. From these findings, radical nitrile-derived fragments under 100 Da are concluded as most heavily responsible for doping/healing of graphene. To further expand the nanobandage method, molecular design of a µm-scale patternable dopant via photolithography is proposed, consisting of a copolymer with a non-doping photocrosslinker and a boron-doping polymer. Foundational work sets the stage to understand the influence of crosslinking on doping via the nanobandage method as well as the effectiveness of patterning, utilizing characterization techniques not available at the nm-scale, which, while often more desired, is difficult to fully characterize, leaving gaps in our knowledge. Further opportunities based on this work are numerous, including the development of additional doping polymers, the expansion of doping/healing techniques to 2D materials beyond graphene, and the application of block copolymers for the nm-scale patterning of multiple dopants simultaneously.