Chemical precipitation at the freezing temperature of~4°C has directly yielded layered rare-earth hydroxide [LRH, Ln 2 (OH) 5-NO 3 ÁnH 2 O, Ln = Y 0.95 Eu 0.05 ] nanosheets (up to 7 nm thick) for the Y/Eu binary system, with the interlayer NO 3 exchangeable with SO 4 2 -. Calcining the sulfate derivative at 1100°C for 4 h produces well-dispersed and readily sinterable Ln 2 O 3 red phosphor powders (~14.8 m 2 /g) that can be densified into highly transparent ceramics via optimized vacuum sintering at the relatively low temperature of 1700°C for 4 h (average grain sizẽ 14 lm; in-line transmittance~80% at the 613 nm Eu 3+ emission or~99% of the theoretical transmittance of Y 2 O 3 single crystal). Our systematic studies also found that (1) the extent of SO 4 2exchange and the interlayer distance of LRH are both affected by the SO 4 2 -/Ln 3+ molar ratio (R), and an almost complete exchange is achievable at R = 0.25 as expected from the chemical formula (one SO 4 2replaces two NO 3 for charge balance). The optimal R value for sintering, however, was found to be 0.03; (2) The Ln 3+ concentration for LRH synthesis substantially affects properties of the resultant oxides, and hard agglomeration has been significantly reduced at the optimized Ln 3+ concentration of 0.05-0.075 mol/L; (3) Sulfate exchange significantly alters the thermal decomposition pathway of LRH, and was found essential to produce well-dispersed and highly sinterable oxide powders; (4) Both the oxide powders and transparent ceramics exhibit the typical red emission of Eu 3+ at 613 nm (the 5 D 0 ? 7 F 2 transition) under charge-transfer (CT) excitation. Red-shifted CT band center, stronger excitation/ emission, and shorter fluorescence lifetime were, however, observed for the transparent ceramics.J. Ballato-contributing editor Manuscript No. 36023.