The strong influence of subsurface heterogeneity on contaminant migration and in situ remediation calls for an improved understanding of its origins and more efficient methods of characterization. Accordingly, an outcrop study of physical and chemical heterogeneity was conducted in a glaciofluvial deposit in Deerfield, New Hampshire, in order to uncover processes controlling the spatial variation of sediment properties and evaluate the extent to which geologic information can be used to characterize the observed variation. The results indicate that physical and chemical properties at the Deerfield site have distinctly different spatial correlation structures. Lithologic facies explain 31% to 60% of the variation in permeability, dithionite citrate (DC)-extractable manganese, and DC-extractable aluminum. Lithofacies bounding surfaces do not separate regions of significantly different DC-extractable iron; instead, 49% of its variation is explained by sediment color. Color also accounts for 34% of the variation in DC-extractable aluminum and 60% of the variation in DC-extractable manganese. Strong relationships with sediment facies and/or color enable detailed mapping of permeability, extractable iron, and extractable manganese. Differences in the geometries of iron and manganese enrichment, petrographic observations, and scanning electron microscope analyses indicate that (hydr)oxide grain coatings originated from the postdepositional weathering of biotite and garnet, coupled with local, redox-driven redistribution of the liberated iron and manganese. The findings suggest that lithofacies and color information can aid the characterization and modeling of heterogeneity at similar carbon-poor glaciofluvial sites.