Dual-pump coherent anti-Stokes Raman scattering (CARS) is used to measure temperature and species profiles in representative non-premixed and partially-premixed CH4/O-2/N-2 flames. A new laser system has been developed to generate a tunable single-frequency beam for the second pump beam in the dual-pump N-2-CO2 CARS process. The second harmonic output (similar to 532 nm) from an injection-seeded Nd:YAG laser is used as one of the narrowband pump beams. The second single-longitudinal-mode pump beam centered near 561 nm is generated using an injection-seeded optical parametric oscillator, consisting of two non-linear beta-BBO crystals, pumped using the third harmonic output (similar to 355 nm) of the same Nd:YAG laser. A broadband dye laser (BBDL), pumped using the second harmonic output of an unseeded Nd:YAG laser, is employed to produce the Stokes beam centered near 607 nm with full-width-at-half-maximum of similar to 250 cm(-1). The three beams are focused between two opposing nozzles of a counter-flow burner facility to measure temperature and major species concentrations in a variety of CH4/O-2/N-2 non-premixed and partially-premixed flames stabilized at a global strain rate of 20 s(-1) at atmospheric-pressure. For the non-premixed flames, excellent agreement is observed between the measured profiles of temperature and CO2/N-2 concentration ratios with those calculated using an opposed-flow flame code with detailed chemistry and molecular transport submodels. For partially-premixed flames, with the rich side premixing level beyond the stable premixed flame limit, the calculations overestimate the distance between the premixed and the non-premixed flamefronts. Consequently, the calculated temperatures near the rich, premixed flame are higher than those measured. Accurate prediction of the distance between the premixed and the non-premixed flames provides an interesting challenge for future computations. (C) 2010 The Combustion Institute. Published by Elsevier Inc. All rights reserved.