There exists a growing body of literature that correlates the fraction of “special” boundaries in a microstructure, as described by the Coincident Site Lattice Model, to properties such as corrosion resistance, intergranular stress corrosion cracking, creep, etc. Several studies suggest that the grain boundary character distribution (GBCD), which is defined in terms of the relative fractions of “special” and “random” grain boundaries, can be manipulated through thermomechanical processing. This investigation evaluates the influence of specific thermomechanical processing methods on the resulting GBCD in FCC materials such as oxygenfree electronic (ofe) copper and Inconel 600. We also demonstrate that the primary effect of thermomechanical processing is to reduce or break the connectivity of the random grain boundary network. Samples of ofe Cu were subjected to a minimum of three different deformation paths to evaluate the influence of deformation path on the resulting GBCD. These include: rolling to 82% reduction in thickness, compression to 82% strain, repeated compression to 20% strain followed by annealing. In addition, the influence of annealing temperature was probed by applying, for each of the processes, three different annealing temperatures of 400, 560, and 800°C. The observations obtained from automated electron backscatter diffraction (EBSD) characterization of the microstructure are discussed in terms of deformation path, annealing temperature, and processing method. Results are compared to previous reports on strainannealed ofe Cu and sequential processed Inconel 600. These results demonstrate that among the processes considered, sequential processing is the most effective method to disrupt the random grain boundary network and improve the GBCD.