Atrazine is the most widely used herbicide in the U.S. and has been detected in surface water and groundwater. Technologies are needed for onsite and in situ remediation of water and soil containing atrazine. We investigated the potential of using fine-grained, zero-valent iron (Fe0) to remove atrazine and promote its degradation in contaminated water and soil. Atrazine loss from aqueous solution increased with increasing Fe0 concentration (w/v). Agitating 20 μg 14C-ring-labeled atrazine L−1 with 10% Fe0 (w/v) removed 92% of the 14C from solution within 48 h. Only about 4% of the 14C lost from solution was extractable from the iron with 3 mM CaCl2 (readily available pool), 81% was extractable with CH3CN (potentially available pool), and 11% was unextractable residues. A companion experiment indicated that most of the 14C extracted from the iron with 3 mM CaCl2 after the 48-h Fe0 treatment was unaltered atrazine, while the CH3CN extract contained approximately 33% atrazine and 48% was unidentified atrazine transformation products. Treating a highly contaminated solution (20 mg atrazine L−1) with 20% Fe0 (w/v) removed 88% of the 14C (added as 14C-ring-labeled atrazine) from solution within 48 h. Deethylatrazine was the main atrazine transformation product detected in solution after treatment, but small amounts of deisopropylatrazine, didealkylatrazine, and hydroxyatrazine were also found. Treating Sharpsburg surface soil containing 1 mg atrazine kg−1 with Fe0 (2%, w/w) increased atrazine mineralization from 4.1 to 11.2% after 120 d. Pyrite (4% FeS2, w/w) also increased atrazine mineralization in surface soil, but was less effective in the presence of NO3− or SO42− (100 mg kg−1 soil). Adding 2% Fe0 (w/w) and 100 mg NO3− kg−1 to contaminated subsurface soil increased atrazine mineralization from 0.4 to 8.2% within 120 d, and unextractable residues increased from 4.6 to 9.8%. These results indicate iron can sorb atrazine and promote its transformation in water and soil.