We present a detailed theoretical study of pressure-broadened Raman line shapes in binary mixtures of nitrogen and carbon monoxide. The semiclassical Robert-Bonamy theory was used to calculate self-broadened Q-branch linewidths of N-2 and CO, and Lennard-Jones (LJ) potential energy surface parameters were fixed by comparing our results with extensive experimental linewidth data. For the case of N-2, the ab initio PES8 potential energy surface was investigated, however, the anisotropic repulsive part had to be reduced to ensure a good agreement with experimental linewidths. The agreement between calculations and experiments was remarkably good, both for self-broadened N-2 and CO Q-branch linewidths. Yet, our calculations were not able to predict the experimentally observed difference between Q- and S-branch linewidths of self-broadened N-2. The central results of this work are the Q-branch linewidths of N-2-CO and CO-N-2, which have been calculated through an extrapolation of the parameters of the potential energy surfaces used for self-broadened linewidths by common combination rules. (C) 2004 American Institute of Physics.