A novel and successful approach to the design of hydrogen-shift, catalysts is presented. Detailed studies of 1-butene hydroisomerization reveal that a catalytic synergism exists in physical mixtures. Mixtures of FeCe/Grafoil and Pt/Grafoil (or Pd/Grafoil) display high selectivity (much greater than Pt) and activity levels as much as ten times larger than the sum of the separately measured activities. Thus, it is demonstrated that highly selective and active isomerization catalysts can be created by physically mixing hydrogen atom generator surfaces (e.g. Pd) with highly selective but low-activity surfaces (e.g. FeCe).