Noachian-aged Jezero crater is the only known location on Mars where clear orbital detections of carbonates are found in close proximity to clear fluvio-lacustrine features indicating the past presence of a paleolake; however, it is unclear whether or not the carbonates in Jezero are related to the lacustrine activity. This distinction is critical for evaluating the astrobiological potential of the site, as lacustrine carbonates on Earth are capable of preserving biosignatures at scales that may be detectable by a landed mission like the Mars 2020 rover, which is planned to land in Jezero in February 2021. In this study, we conduct a detailed investigation of the mineralogical and morphological properties of geological units within Jezero crater in order to better constrain the origin of carbonates in the basin and their timing relative to fluvio-lacustrine activity. Using orbital visible/near-infrared hyperspectral images from the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) along with high resolution imagery and digital elevation models, we identify a distinct carbonate-bearing unit, the “Marginal Carbonates,” located along the inner margin of the crater, near the largest inlet valley and the western delta. Based on their strong carbonate signatures, topographic properties, and location in the crater, we propose that this unit may preserve authigenic lacustrine carbonates, precipitated in the near-shore environment of the Jezero paleolake. Comparison to carbonate deposits from terrestrial closed basin lakes suggests that if the Marginal Carbonates are lacustrine in origin, they could preserve macro- and microscopic biosignatures in microbialite rocks like stromatolites, some of which would likely be detectable by Mars 2020. The Marginal Carbonates may represent just one phase of a complex fluvio-lacustrine history in Jezero crater, as we find that the spectral diversity of the fluvio-lacustrine deposits in the crater is consistent with a long-lived lake system cataloging the deposition and erosion of regional geologic units. Thus, Jezero crater may contain a unique record of the evolution of surface environments, climates, and habitability on early Mars.