A combination of techniques, including AES, SIMS, FTIR, and hydrogen chemisorption, has been used to investigate the activation of nickel ions supported on hydrous titanium oxide (HTO) ion-exchange materials.H T O supports allow metal ions to be loaded via ionvexchange such that atomic dispersion is attained in the as-prepared material, even for high metal loadings. The results presented here support earlier work indicating that nickel forms large, 10-20-nm particles during hydrogen reduction of N i / H T O at temperatures of 300 "C or greater. During reduction, these particles become covered by an amorphous film which inhibits catalytic activity. Evidence is presented which supports the theory that this film is composed of carbonaceous residue which originates from the organometallic precursors and organic solvents used to synthesize the H T O support. Reduction/oxidation cycles result in oscillations in the nickel surface concentration which are attributed to decoration of the particles by partially reduced TiO, species, in a manner similar to a strong metal-support interaction (SMSI). This SMSI occurs at temperatures as low as 300 O C , well below the temperatures typically required to induce SMSI on crystalline titania supports. This low onset temperature appears to be related to the amorphous nature of the H T O support, which may be more easily reduced than crystalline titania. Mild oxidation.(300 "C) of N i / H T O prior to reduction increases the amount of metal surface area which is formed during reduction by altering the interaction of the nickel ions with the support such that smaller nickel particles are formed. More severe oxidation treatments (>400 "C) lead to a decrease in active surface area by increasing the interaction of nickel ions with the support such that a smaller fraction of the nickel ions can be reduced and participate in particle formation.