In this study, TiO2-polyvinyl alcohol (PVA) composite granules were prepared via spray drying technique. To investigate the effects of solid content and binder/powder ratio in the slurry on the granulation behavior of TiO2 powders, the feed compositions were designed to vary over a wide range. The morphology, actual densities, and average granule size and size distribution of the TiO2-PVA composite granules were characterized by using scanning electron microscopy technique, a gas pycnometer, and an image analyzing program (Image-J), respectively. The results indicate that solid content and the amount of PVA in the feedstock slurry are the dominant factors determining the granule morphology, size, and size distribution of TiO2-PVA composite. Moreover, it was observed that increasing the solid content and the amount of PVA in the slurry improved the granulation process and reduced the granule defects. For the preparation of spherical TiO2-PVA composite granules with the minimum amount of non-granulated powders, the optimized composition of the feedstock slurry was found to be 35 wt.% solid and 3 wt.% PVA.