Atomic force microscopy (AFM) is a nanoscale scanning probe microscopy (SPM) characterization technique useful for obtaining topographical maps of surfaces and their associated nanomechanical properties. Complementary SPM modes such as Kelvin probe force microscopy (KPFM) and magnetic force microscopy (MFM) can simultaneously elucidate the electrical and magnetic properties of materials with nanoscale resolution, thereby expanding AFM’s utility. KPFM measures the Volta potential difference between a conductive AFM probe and the sample surface, which can be related back to the work function of the material and correlated with co-localized elemental mapping via energy dispersive spectroscopy (EDS). This can be useful for understanding and predicting initiation and propagation of galvanic corrosion in metal alloys. MFM employs a magnetized AFM probe tip to detect magnetic interactions between the sample and the tip, thereby mapping out the magnetic structure of the sample surface. Here we present KPFM studies of case-hardened stainless steels engineered for bearing applications in high performance jet engines destined for operation in corrosive marine environments. MFM studies of Ni-Mn-Ga, a magnetic shape memory alloy, connect experimental data with computational modeling to understand the growth of twins in response to bending. Together, these studies highlight the widespread applicability of AFM, KPFM, MFM, and other SPM techniques for illuminating nanoscale structure-property relationships in material systems.