The hydrogenolysis of methylcyclopentane and the isomerization of 2-methylpentane were studied over Pt-Ru bimetallic catalysts prepared using either H2PtCl6 and RuCl3 (Series A) or from Pt(NH3)(4)(NO3)(2) and Ru(NH3)(6)Cl-3 (Series B). Energy-dispersive X-ray spectroscopy (EDXS) studies showed that the catalysts prepared using the amine precursors were 100% bimetallic. Image defocussing studies suggest that approximately 20% of the particles prepared using the chloride precursors were monometallic, At temperatures at which only ruthenium is active (413 K), the formation of C-1 to C-5 products was depressed over Pt-Ru bimetallic clusters, Tertiary-secondary carbon-carbon bond cleavage approaches that observed for ruthenium while secondary-secondary carbon-carbon bond cleavage is closer to that observed for platinum, The isomerization of 2MP at 493 K is representative of Pt-Ru activated dual sites since platinum is inactive at this temperature and ruthenium leads to extensive degradation of the molecule. The contribution of the cyclic mechanism was obtained using C-13 labelled species. A synergistic effect was observed for the catalysts prepared using amine precursors. This is explained by considering an increase in the number of PtRu dual surface sites.