Carbon subsurface concentration profiles in olivine single crystals from San Carlos, Arizona, and the Sergebet Island. Red Sea, containing total carbon between 60–180 wt.-ppm, were analyzed by means of the 12C(d. p) 13C nuclear reaction and by x-ray induced photoelectron spectroscopy (XPS) in combination with acid etching and with Ar + ion sputtering respectively, between 200–930 K. The (d, p) analysis reveals equilibrium subsurface C profiles extending 1–2 μm or more into the bulk. Their steepness is a function of temperature. Typical mean C concentrations at 300 K in the resolvable layers, 0–0.6, 0.6–1.2, and 1.2–1.8 μm. are 1.8, and 0.6 wt.-%, corresponding to enrichment factors over the mean bulk C concentration of the order of 100, 40 and 30 respectively. In the topmost atomic layers analyzed by XPS the carbon is enriched by a factor of the order of 1000, decreasing with increasing temperature. The results suggest that the carbon is in a truly dissolved state and highly mobile, subject to a reversible subsurface segregation. Most probably local lattice strain associated with the solute C species provide the driving force for this diffusional process. The C diffusion coefficient was determined from the (d, p) data below 300 K: D= 10 −13 exp(−7.8/RT) [m 2· sec −1; KJ · mole −1] and from XPS data between 450–925 K: D = 10 −14 exp(-6/RT) [m 2 · sec −1; KJ · mole −1] The estimated error of the preexponential factors is ± one order of magnitude, that of the activation energies ±3.5 and ±2 KJ mole −1 respectively.