The aim of this study was to investigate the preparation of co-amorphous mixture-layered pellets using solventless pelletization and amorphization using a high shear granulator (as suggested in the first part of this study) by high shear mixing of drug crystals and a crystalline co-former with inactive spheres. Mixtures of crystalline indomethacin and arginine at various molar ratios were mixed with microcrystalline cellulose spheres at a weight ratio of 1:10 using the granulator and the resulting particles were characterized using solid-state and particle analytical techniques as well as dissolution testing and physical stability. At jacket temperatures of 20 °C or more of the granulator, co-processing of indomethacin and arginine enhanced amorphization of indomethacin and provided a co-amorphous mixture due to homogenous mixing of indomethacin and arginine amorphous phases. The co-amorphous mixture was deposited on the surface of the spheres, yielding co-amorphous mixture-layered pellets. The co-amorphous mixtures at molar ratios of indomethacin to arginine of 2:1 and 1:1, deposited on the pellets, did not recrystallize for at least 4 weeks. The pellets exhibited higher dissolution characteristics as additional hypromellose could prevent precipitation. These findings demonstrate the potential of this technique as a solventless approach to prepare co-amorphous mixture-layered pellets through a one-step process.