LaZrOx- or YZrOx-based catalysts with supported Rh, Ru, Pt, or Ir nanoparticles were tested in the nonoxidative dehydrogenation of isobutane to isobutene (IsoBDH). For each supported metal, there is an optimum loading to achieve the highest activity. This is due to the different abilities of the metals to promote the formation of catalytically active Zr-cus (cus means coordinatively unsaturated) through removal of lattice oxygen from ZrO2 upon reductive catalyst treatment. The kind of supported metal is also decisive for skeletal isomerization, with Rh and Pt showing the lowest and the highest activity, respectively. An isobutene selectivity of about 96% can be achieved at an isobutane conversion of about 35% at 550 degrees C. Under such conditions, Rh(0.05 wt %)/YZrOx revealed the highest space-time yield of isobutene formation of 2.7 kg(isobutene).kg(catalyst)(-1).h(-1). The ratio of isobutene/n-butenes was above 3000. This catalyst was also durable over 40 dehydrogenation/regeneration cycles.