An analysis of structure in rotation measure (RM) across the sky based on the RM catalog of Taylor et al. (2009) is presented. Several resolved RM structures are identified with structure in the local ISM, including radio loops I, II, and III, the Gum nebula, and the Orion-Eridanus super bubble. Structure functions (SFs) of RM are presented for selected areas, and maps of SF amplitude and slope across the sky are compared with Hα intensity and diffuse polarized intensity. RM variance on an angular scale of 1 • is correlated with length of the line of sight through the Galaxy, with a contribution from local structures. The slope of the SFs is less concentrated to the Galactic plane and less correlated with length of the line of sight through the Galaxy, suggesting a more local origin for RM structure on angular scales ∼ 10 • . The RM variance is a factor ∼ 2 higher towards the SGP than towards the NGP, reflecting a more wide-spread asymmetry between the northern and southern Galactic hemispheres. Depolarization of diffuse Galactic synchrotron emission at latitudes < 30 • can be explained largely by Faraday dispersion related to small-scale variance in RM, but the errors allow a significant contribution from differential Faraday rotation along the line of sight.