We have identified terrestrial sources of methyl iodide (CH3I) and assessed their importance in its atmospheric budget using a synthesis of field observations. Measurements include those from NASA DC‐8 research flights over the United States and the North Atlantic, the AIRMAP long‐term ground‐observing network in New England, and a field campaign at Duke Forest, North Carolina. We found an average CH3I flux of ∼2,700 ng m−2 d−1 to the atmosphere from midlatitude vegetation and soils, a value similar in magnitude to previous estimates of the oceanic source strength. The large‐scale aircraft measurements of vertical profiles over the continental U.S. showed CH3I‐mixing ratios comparable to and greater than those observed over the North Atlantic. Overall, midlatitude terrestrial biomes appear to contribute 33 Gg yr−1 to the CH3I global budget.