We performed laboratory laser-induced breakdown spectroscopy (LIBS) and laser Raman spectroscopy measurements on samples from a layered outcrop from the Atacama Desert, Chile. This outcrop is a terrestrial morphological and possibly mineralogical analogue for similar formations that will likely be investigated by the Curiosity rover at Gale Crater. Our results demonstrate that fast LIBS analysis can generate semiquantitative chemical profiles in subminute times using automated data processing tools. Therefore, the LIBS instrument can be an invaluable tactical tool on the Curiosity rover for remote, rapid geochemical survey of layered outcrops, thus serving daily operational needs. The derived chemical profiles, supported by the range of minerals identified by Raman spectroscopy, is consistent with the products of a continental evaporitic lake. In the framework of future surface exploration on Mars, a combined Raman/LIBS investigation may provide a rapid mineralogical/chemical evaluation of targets that can be useful for selecting samples to be eventually collected for sample return purposes or for selecting sample sites to be drilled in the search for astrobiology-relevant species.