The Cloud Physics LiDAR (CPL) WHyMSIE dataset consists of backscatter coefficient, lidar depolarization ratio, layer top/base height, layer type, particulate extinction coefficient, ice water content, and layer/cumulative optical depth data collected from the Cloud Physics LiDAR (CPL) onboard the NASA ER-2 high-altitude research aircraft in support of the Westcoast and Heartland Hyperspectral Microwave Sensor Intensive Experiment (WHyMSIE) field campaign. WHyMSIE aimed to capture a wide variety of thermodynamic, moisture, and planetary boundary layer regimes across a variety of surface types. Comparing observations from CPL, other instruments, and with in situ observations of temperature and humidity will allow for scientific advancement of remote-sensing techniques into the hyperspectral microwave era and improved understanding of the planetary boundary layer at different measurement scales. The dataset files are available in HDF-5 format from October 18, 2024, through November 13, 2024.