The objective of this study was to compare mid-infrared (MIR) an near-infrared (NIR) spectroscopy (MIRS and NIRS, respectively) not only to measure soil carbon content, but also to measure key soil organic C (SOC) fractions and the delta13C in a highly diverse set of soils while also assessing the feasibility of establishing regional diffuse reflectance calibrations for these fractions. Two hundred and thirty-seven soil samples were collected from 14 sites in 10 western states (CO, IA, MN, MO, MT, ND, NE, NM, OK, TX). Two subsets of these were examined for a variety of C measures by conventional assays and NIRS and MIRS. Biomass C and N, soil inorganic C (SIC), SOC, total C, identifiable plant material (IPM) (20x magnifying glass), the ratio of SOC to the silt+clay content, and total N were available for 185 samples. Mineral-associated C fraction, delta13C of the mineral associated C, delta13C of SOC, percentage C in the mineral-associated C fraction, particulate organic matter, and percentage C in the particulate organic matter were available for 114 samples. NIR spectra (64 co-added scans) from 400 to 2498 nm (10-nm resolution with data collected every 2 nm) were obtained using a rotating sample cup and an NIRSystems model 6500 scanning monochromator. MIR diffuse reflectance spectra from 4000 to 400 cm-1 (2500 to 25,000 nm) were obtained on non-KBr diluted samples using a custom-made sample transport and a Digilab FTS-60 Fourier transform spectrometer (4-cm-1 resolution with 64 co-added scans). Partial least squares regression was used with a one-out cross validation to develop calibrations for the various analytes using NIR and MIR spectra. Results demonstrated that accurate calibrations for a wide variety of soil C measures, including measures of delta13C, are feasible using MIR spectra. Similar efforts using NIR spectra indicated that although NIR spectrometers may be capable of scanning larger amounts of samples, the results are generally not as good as achieved using MIR spectra.