Abstarct: Among engineering ceramics Alumina enjoys unique properties such as high resistance to fatigue, wear and corrosion along with high hardness. However, it suffers from low toughness. An effective method to enhance the toughness of Alumina is to use second-phase, tetragonal Zirconia. Reinforcing ceramics with Carbon nanotubes (CNT) can result in tough ceramic composites with high hardness and thermal stability. Among methods of producing Zirconia toughened Alumina with multiwall Carbon nanotubes (ZTA–MWCNT), tape casting stands out not only as among the most cost-effective, but also as able to produce composite thin films. In this study we sought to produce ZTA–MWCNT composite thin films and to examine their properties. Dolapix PC21, Sodium Dodecyl Sulfate (SDS) and Polyvidone (PVP) were used separately as dispersants agents. Green tapes were pre-fired at 500 ℃ for two hours, and sintered at 1,400 ℃ and 1,600 ℃ for two and seven hours each. Mean hardness of 28 ± 1 GPa for measurements from 0.01 wt. % MWCNT samples sintered for seven hours at 1,600 ℃ were obtained and outstanding highest Vickers hardness test result is 47.33 GPa. This is respectively 64% and 121% higher than mean and highest reported values from ZTA- MWCNT composite samples; regardless of preparation and sintering methods. X-ray diffraction test confirmed the existence of Alumina and tetragonal Zirconia in these samples while scanning electron microscope (SEM) images showed grain fining, homogeneity of the composite structure, high final density and proper sintering. These images also show the fracture surfaces of the pulled-out MWCNT. Rheology test of the aqueous slurry confirmed shear thinning behavior and viscosity of 1.76 Pa. s under shear rate of 1,000 s–1, making the slurry ideal for tape casting.