Mullite is widely used as a structural material for applications like thermal and environmental barriers coatings. For some of these applications, thermal spray is a suitable technique due to its fast production time and versatility. This makes mullite a very interesting coating material for thermal spray industry. In the present work, the viability to produce coatings by thermal spray using mullite-CNFs agglomerated powders is analyzed. The stability of aqueous mullite and mullite-CNFs suspensions was studied in terms of zeta potential and rheological behaviour of concentrated slurries. Slurries were optimized in terms of dispersant concentration and solid content. The optimized suspensions were used for the granules preparation by spray drying technology. The obtained granules were characterized through the determination of particle size distribution and shape factor by field emission scanning electron microscopy and laser scattering. These granules were used to form the coatings by Atmospheric Plasma Spraying which were characterized by evaluating the composition, structure, shape, and thickness.