This work concerns the use of parallel electron energy loss spectroscopy (PEELS) to investigate the detection, distribution, and quantification of carbon in various steel microstructures generated by rapid cooling rates or by isothermal transformation. The feasibility of detecting C in steels containing very small amounts of carbon was first examined by calculating the minimum detectable mass fraction for a variety of binary Fe-C alloy specimen thicknesses and microscope conditions. These theoretical studies indicated that the detection of carbon in steel microconstituents containing about 0.01 wt.% (or even less) was easily possible with an analytical transmission electron microscope equipped with a LaB6 emitter and a PEEL spectrometer. These theoretical calculations seemed to be reasonable, as it proved possible to make a quantitative PEELS study of the partitioning between the microconstituents ferrite, retained austenite, and martensite found in an ultralow carbon (0.03 wt.%) steel weld metal provided care was taken to avoid hydrocarbon contamination. Studies of both carbon and molybdenum segregation to ferrite/martensite interfaces in an isothermally transformed Fe-C-Mo alloy were also carried out in order to investigate the nature of the “solute drag” effect in this alloy system.