Cyanide bridged lanthanide-palladium transition metal complexes were employed as catalyst precursors in the catalytic reduction of NO with methane. Complexes {(DMF)(10)Ln(2) [Pd(CN)(4)](3)}(infinity) (Ln = Yb, Sm; DMF = dimethyl formamide) were dispersed (10 wt.% loading based upon palladium) on sol-gel titania supports and reduced by ammonia or hydrogen to metallic nanoparticles containing palladium and lanthanide metals. They were tested for catalytic activity in NO reduction by CH4 in the presence of oxygen. The bimetallic catalysts were found to be active for NO reduction up to the stoichiometric oxygen concentrations. They displayed improved performance over a palladium only catalyst. Catalysts were examined by TEM, and XPS techniques before, during, and after the reaction.