A rapid image segmentation and correlation-based approach to investigating the local microstructural effects on pitting corrosion susceptibility is introduced. The impact of four different microstructural features, consisting of grain orientation, proximity to grain boundaries, proximity to intermetallic particles, and local geometrically necessary dislocation (GND) density, on pitting initiation in the 5083 aluminum alloy was directly investigated using automated pit detection processing in combination with electron microscopy-based characterization. Three different thermomechanical treatments were used to vary the system microstructure and samples were immersed in 3.5 wt% NaCl aqueous solution for 24 h to induce pitting. GND density and proximity to intermetallic particle both showed positive correlations, while grain orientation and proximity to grain boundary showed no correlation with pit initiation sites.