Laboratory studies were conducted to quantify and understand the processes by which iodide (I-) adsorbs to subsurface arid sediments. A surprisingly large amount of I- sorbed (distribution coefficients [Kd?s] ranged from 1 to 10 mL/g and averaged 3.3 mL/g) to three alkaline subsurface sediments that were low in organic matter content. Experiments with pure mineral isolates, similar to the minerals identified in the clay fraction of the sediments, showed that there was little or no I- sorption. The pure minerals that had low iodide sorption include montmorillonite (Kd = -0.42 +/- 0.08 mL/g), quartz (Kd = 0.04 +/- 0.02 mL/g), vermiculite (Kd = 0.56 +/- 0.21 mL/g), calcite (Kd = 0.04 +/- 0.01 mL/g), goethite (Kd = 0.10 +/- 0.03 mL/g), or chlorite (Kd = -0.22 +/- 0.06 mL/g). Conversely, a significant amount of I- sorbed to illite (Kd = 15.14 +/- 2.84 mL/g). Upon treating the iodide-laden illite with dissolved F-, Cl-, Br-, or I-127, desorption (or isotopic exchange in the case of I-127) removed, respectively, 57 +/- 3%, 55 +/- 0%, 48 +/- 3, and 17 +/- 1% of the I- originally adsorbed to the illite. The fact that such large amounts of I- could be desorbed suggestsmore » that the I- was weakly adsorbed, and not chemically bonded to a soft metal, such as mercury or silver, that may have existed in the illite structure as trace impurities. Finally, I- sorption to illite was strongly pH-dependent; the Kd values decreased from 46 to 22 mL/g as the pH increased from 3.6 to 9.4. Importantly, I- sorbed to illite even under alkaline conditions. Together, these experiments suggest that illite removed I- from the aqueous phase predominantly by reversible physical adsorption to the pH-dependent edge sites. Illites may constitute a substantial proportion of the clay-size fraction of many arid sediments and therefore may play an important role in retarding I- movement in these sediments.« less