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0–3 type ferroelectric–phosphor composite ceramics cannot be prepared by the traditional solid-state sintering (SSS) method due to the strong chemical reaction between ferroelectrics and phosphors during high-temperature sintering. The cold sintering process (CSP) may solve this issue by densifying ceramics at ultralow sintering temperatures. In this work, dense 0–3 type 0.8BaTiO3–0.2CaTiO3:Pr3+ (0.8BT–0.2CT:Pr3+) binary composite ceramics were fabricated at an ultralow temperature of 225 °C via CSP with the Ba(OH)2·8H2O hydrated flux. The effects of the Ba(OH)2·8H2O content, sintering temperature, and sintering time on the microstructure and densification of the ceramics were investigated. The density of the composite ceramics prepared by the optimized sintering parameters reaches 89%. Both energy-dispersive X-ray (EDX) spectroscopy and X-ray diffraction (XRD) confirm the existence of BT and CT:Pr3+ phases in the prepared ceramics. A strong ferroelectric performance is obtained, and the luminescent properties of CT:Pr3+ are preserved for the ceramics. Furthermore, the 0.8BT–0.2CT:Pr3+ composite ceramics prepared by CSP have stronger photoluminescence and photo-stimulated luminescence than their counterparts prepared by cold sintering assistance (CSA) and SSS methods. Therefore, CSP is a promising method for combining luminescent and ferroelectric properties into 0–3 type composite ceramics.
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