The compositional, thermophysical and geologic characteristics of surface units in Iapygia and Tyrrhena Terra (60°E–100°E, 0°–30°S) provide new insights into the compositional stratigraphy of the region. Intercrater plains are dominated by two surface units. The older unit (unit 1) is deficient in olivine and more degraded and likely consists of a mixture of impact, volcanic and sedimentary materials. The younger unit (unit 2) is enriched in olivine, exhibits a resistant morphology and higher thermal inertia, and likely represents volcanic infilling of plains. Units 1 and 2 bear a strong resemblance to those previously mapped in Mare Serpentis, a section of highlands crust located northwest of Hellas Basin. Thus, the two major intercrater plains units are even more widespread than previously thought and therefore likely constitute important components of Mars' highland stratigraphy. Many craters in the region contain high thermal inertia deposits (unit 3) that are compositionally identical to unit 2. These may have formed via volcanic infilling or may represent sedimentary materials that have been eroded from crater walls and lithified. Less common units include olivine and/or pyroxene‐rich massifs and crater central peaks. These are primarily found within Hellas Basin rim units and may represent mantle materials brought toward the surface during the Hellas impact. Putative chloride deposits are primarily associated with olivine‐deficient surfaces (unit 1) that may be heavily degraded occurrences of unit 2. The observations raise a variety of questions related to Martian crustal evolution and alteration that may have more widespread implications outside the study region.