The production of H2 has been examined in the gamma-ray and 5 MeV He ion radiolysis of CaCl2.2H2O, CaCl2.6H2O, Ca(OH)2, MgCl2.2H2O, MgCl2.6H2O, and Mg(OH)2. The highest yield for the formation of H2 is observed in the gamma-radiolysis of MgCl2.2H2O (0.72 molecule/(100 eV), 75 nmol/J), but the yield decreases with dose due to the relative instability of the dihydrate. The H2 yields with the other compounds range from 0.04 to 0.2 molecule/(100 eV) (4.2-21 nmol/J), which is lower than that from pure water or 2 M chloride solutions. There appears to be no relationship between the results for H2 from waters of hydration with that from aqueous salt brines. No particular trend is observed in the radiation chemical yields of H2 with respect to the cation or the degree of hydration. The production of Cl2 is found only in the gamma-radiolysis of CaCl2 with a few weight percent of excess water. No Cl2 was found in the 5 MeV He ion radiolysis of identical systems. None of the other compounds examined here showed detectable amounts of Cl2 formation.