Ag-containing aluminosilicate sorbents capable of capturing iodine were prepared by sol-gelation from Na, Al, and Si alkoxides using co-solvent exchange, Ag/Na ion exchange, solvent exchange, and ambient-pressure drying. The Na+AlSi-OH gel was prepared using sodium methoxide (NaOMe): aluminum tri-sec-butoxide (Al(OsBu)3): tetraethyl orthosilicate (TEOS) molar ratios of 1.05:1:1, 1.3:1.1:1, 1.5:1.3:1. The solvent effect on textural properties such as Brunauer-Emmett-Teller (BET) surface areas and pore size distributions and Ag0 particle sizes was investigated using water with high surface tension, isopropanol and n-heptane with low surface tension. The BET surface area, average pore size, and cumulative pore volume for sorbents strongly increased with decreasing surface tension of solvents and increasing Al/Si atomic ratios. In addition, Ag0 particle sizes increased with decreasing surface tension of solvents.