The Microwave Limb Sounder on Aura has produced an extensive set of measurements of CO in the middle atmosphere. The measurements are usable for scientific studies from the upper troposphere up to 90 km altitude. We describe these measurements and validate them by demonstrating their internal consistency and by comparing them to other remotely sounded measurements and to 2-D model simulations. Comparisons with other measurements suggest that MLS has a positive bias of 25–50% in the mesosphere and a negative bias of up to 70% in the (almost CO-free) lower stratosphere. The geophysical features observed in the MLS CO field show excellent qualitative agreement with other measurements.