AbstractWe have measured the CO2 volume mixing ratio (VMR) within the planetary boundary layer (PBL) using cloud slicing with an airborne pulsed integrated path differential absorption (IPDA) lidar from flight altitudes of up to 13 km. During a flight over Iowa in summer 2011, simultaneous measurement of the optical range and CO2 absorption to clouds and the ground were made using time‐resolved detection of pulse echoes from each scattering surface. We determined the CO2 absorption in the PBL by differencing the two lidar‐measured absorption line shapes, one to a broken shallow cumulus cloud layer located at the top of the PBL and the other to the ground. Solving for the CO2 VMR in the PBL and that of the free troposphere, we measured a ≈15 ppm (4%) drawdown in the PBL. Both CO2 VMRs were within ≈3 ppm of in situ CO2 profile measurements. We have also demonstrated cloud slicing using scatter from thin, diffuse cirrus clouds and cumulus clouds, which allowed solving for the CO2 VMR for three vertical layers. The technique and retrieval algorithm are applicable to a space‐based lidar instrument as well as to lidar IPDA measurements of other trace gases. Thus, lidar cloud slicing also offers promise toward space‐based remote sensing of vertical trace gas profiles in the atmosphere using a variety of clouds.