Laminated sandstones from the 2.9 Ga Pongola Supergroup, South Africa, were characterized using micro-Raman spectral imaging to elucidate the origin of the mineral components. These sandstones were formed in a paleoenvironment conducive to sustaining life and contain compelling features reminiscent of ancient microbial mat remains. Most sedimentary rocks of this age have been altered over time through metamorphism and weathering, obscuring any original biologic or mineralogic signatures. Therefore, determination of the exact formation mechanism for biologically associated features is often precluded, resulting in large gaps in our understanding of early life and Earth's early habitable environments. The results of the Raman analyses show that the parallel to bedding laminations in these rocks consist of elongated muscovite grains that are intimately associated with anatase, rutile, goethite, and graphitic carbon. The morphology, orientation, and intimate associations of the component mineral assemblage in the laminations suggest that physiochemical events, such as weathering, low-grade metamorphism, or hydrothermal fluids, were also key in their formation and influenced their geochemical makeup. Given the complicated histories of ancient sedimentary rocks, the use of techniques such as micro-Raman spectroscopy is crucial in determining the origins of sedimentary structures that might otherwise be misinterpreted. Copyright © 2011 John Wiley & Sons, Ltd.