We present time-domain measurements and modelling of the CH4 nu(1) vibrational Q-branch, as well as simultaneous temperature acquisition from the CH4 and N-2 vibrational Q-branches using broadband hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS). Accurate measurements with fs/ps CARS require knowledge of the time-domain response of the probed molecule at different temperatures and pressures. In this work, a fs/ps CARS model was developed for the CH4 nu(1) Q-branch and validated using time-resolved probe delay scans at pressures between 70 and 600 Torr and temperatures between 295 and 1000 K. A simplified modified exponential energy gap model was used to determine the linewidths of the Raman transitions within the Q-branch. Total Q-branch linewidths for the entire explored parameter space were also determined from the probe delay scans. This enabled quantitative measurements of CH4 with fs/ps CARS as well as the temperature through the hot bands of the CH4 nu(1) Q-branch. With a broadband fs laser pulse in a two-beam phase matching scheme, the N-2 Q-branch and CH4 nu(1) Q-branch were simultaneously measured in a heated cell, and the temperatures from each molecule's spectra was evaluated. The fitted temperatures corresponded well with differences ranging from 4 to 17%. It was also shown that exchanging 90% of CH4 for N-2 or Ar at 295 K and 500 Torr did not significantly impact the normalized time-domain signal prior to a 100 picosecond probe delay. Spatially resolved one-dimensional (1-D) thermometry using the CH4 Q-branch was also demonstrated with an imaged spatial resolution of 40 pm. With the developed model, 1-D quantitative measurements of CH4 concentration and temperature can be measured with time resolution of tens of picoseconds. (C) 2020 The Combustion Institute. Published by Elsevier Inc. All rights reserved.