This dataset provides atmospheric carbon dioxide (CO2), carbon monoxide (CO), and methane (CH4) concentrations as measured on a network of instrumented communications towers operated by the Atmospheric Carbon and Transport-America (ACT-America) project. ACT-America's mission spans five years and includes five 6-week intensive field campaigns covering all 4 seasons and 3 regions of the central and eastern United States. Tower-based measurements began in early 2015 and are continuously collecting CO2, CO, and CH4 data to characterize ground-level (>100 m) carbon background conditions to support the periodic airborne measurement campaigns and transport modeling conducted by ACT-America. The towers are instrumented with infrared cavity ring-down spectrometer systems (CRDS; Picarro Inc.). Data are reported for the highest sampling port on each tower. The averaging interval standard deviation and uncertainty derived from periodic flask sample to in-situ measurement comparisons are provided. Complete tower location, elevation, instrument height, and date/time information are also provided.