Based on X-ray photoelectron spectroscopy and X-ray diffraction data for zinc oxide powders prepared via mechanical milling in an attritor, we have identified inherent features of the chemical binding of carbon dioxide on the surface of the powders. The results thus obtained can be used in the fabrication of carbon dioxide sensors, catalysts, and photocatalysts with improved performance parameters. The powders milled for 3 h exhibit the most active interaction with atmospheric carbon dioxide and have the largest percentage of carbon chemisorbed in carbonate-like form.