Uncrewed Systems (UxS), including uncrewed aerial systems (UAS) and tethered balloon/kite systems (TBS), are significantly expanding observational capabilities in atmospheric science. Rapid adaptation of these platforms and the advancement of miniaturized instruments have resulted in an expanding number of datasets captured under various environmental conditions by the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility. In 2021, observational data collected using ARM UxS platforms, including seven TigerShark UAS flights and 133 tethered balloon system (TBS) flights, were archived by the ARM Data Center (https://adc.arm.gov/discovery/#/, last access: 11 February 2022) and made publicly available at no cost for all registered users (https://doi.org/10.5439/1846798) (Mei and Dexheimer, 2022). These data streams provide new perspectives on spatial variability of atmospheric and surface parameters, helping to address critical science questions in Earth system science research. This paper describes the DOE UAS/TBS datasets, including information on the acquisition, collection, and quality control processes, and highlights the potential scientific contributions using UAS and TBS platforms.