Zirconia-toughened alumina (ZTA) powders with 20.0 wt.% of ZrO2 were synthesized using the coprecipitation method. Transmission electron microscopy indicated that the powders contained needle-like particles 15–30 nm long and 50–70 nm flake-like particles with a uniform component distribution. Effects of different Y2O3 concentrations (3.0, 4.0, or 5.0 mol.%) and 0.5 wt.% of MnO on the phase composition, microstructure, and physicomechanical properties of the composites were evaluated after sintering at 1600 °C. The microhardness of 5ZTA-Mn samples (5.0 mol.% of Y2O3 and 0.5 wt.% of MnO) was 1653 ± 50 HV when density reached 4.18 g/cm3. For digital light processing on a commercial 3D printer Anycubic Photon S, acrylate-based homogeneous slurries were obtained. Compositions based on ZTA powder stabilized with 5.0 mol.% of Y2O3 and containing 0.5 wt.% of MnO were studied. MnO in the materials improved polymerization depth during the UV-curing process as compared to 5ZTA materials. The microstructure and mechanical properties of the 5ZTA-Mn composites were investigated at the sintering temperature of 1600 °C. Compared with 5ZTA, the 5ZTA-Mn composites showed higher density (4.0 g/cm3) and microhardness (1409 ± 50 HV). According to in vitro experiments, the newly developed materials are promising for biomedical applications and can serve as a basis for the production of personalized implants via digital light processing printing.