Fourier-transform laser Raman spectroscopy in the near infrared (1064 nm) has been used to characterize a variety of key pigments and biomolecules produced by cyanobacteria and other stress-tolerant microbes in material from extreme Antarctic cold deserts analogous to martian habitats. These compounds include photosynthetic pigments and sunscreens to protect against harmful UV radiation in the light zone (chlorophyll, scytonemin, β-carotene) and photoprotective minerals, such as silica containing iron (III) oxide. Calcium oxalate mono- and dihydrate produced as a result of the biological weathering processes and stress-protective compounds, necessary to protect organisms against desiccation, freezing temperatures, and hypersalinity, such as water-replacement molecules (trehalose), are also monitored. From the results obtained using Antarctic samples, it is shown that a laser-based system can be used to characterize biomolecules in their natural state within their mineral microhabitats. Because of the similarities between the Antarctic cold desert ecosystems, which represent some of the most extreme terrestrial environmental habitats, and putative martian analogs, the laser-Raman spectrosocopic approach is proposed for the detection of former life on Mars analogs to terrestrial cyanobacteria under stress, such as stromatolites, evaporites, and endolithic communities. To this end, the spectral database that is being accumulated from laser-Raman studies of these Antarctic communities will provide a resource of potential biomarkers for future remote laser-Raman analysis on future Mars missions.