Recalibrated and geometrically registered multispectral images from the Imager for Mars Pathfinder (IMP) were analyzed using Spectral Mixture Analysis (SMA) and related techniques. SMA models a multispectral image scene as a linear combination of end-member spectra, and anomalous materials which do not fit the model are detected as model residuals. While most of the IMP data studied here are modeled generally well using "Bright Dust," "Gray Rock," and "Shade" image endmembers, additional anomalous materials were detected through careful analysis of root mean square (RMS) error images resulting from SMA. For example, analysis of SMA fraction and RMS images indicates spectral differences within a previously monolithologic Dark Soil class. A type of Dark Soil that has high fractional abundances in rock fraction images (Gray Rock Soil) was identified. Other anomalous materials identified included a previously noted "Black Rock" lithology, a class of possibly indurated, compacted, or partially cemented soils ("Intermediate Soil"), and a unit referred to as "Anomalous Patches" on at least one rock. The Black Rock lithology has a strong 900-1000-nm absorption, and modeling of the derived image endmembers using a laboratory reference endmember modeling (REM) approach produced best-fit model spectra that are most consistent with the presence of high-Ca pyroxenes and/or olivine, crystalline ferric oxide minerals, or mixtures of these materials as important components of the Black Rock endmember. More unique mineralogic identifications could not be obtained using our initial REM analyses. Both Intermediate Soil and Anomalous Patches units exhibit a relatively narrow 860-950-nm absorption that is consistent with the presence of either low-Ca pyroxenes or a cementing crystalline ferric oxide mineral. ?? 2002 Elsevier Science (USA).