Single-crystal, submicrometer-sized CaS:Eu luminescent particles were synthesized via a solvothermal route, and these moisturesensitive particles were coated with aluminum oxide using atomic layer deposition ͑ALD͒. Photoluminescence ͑PL͒ spectra of coated and uncoated particles were compared. They both showed a broad-band PL emission with a maximum of 650 nm. Microencapsulation by aluminum oxide layers did not have a pronounced effect on the intensity of the emission. In situ luminescence measurements during the accelerated aging ͑80°C, 80% relative humidity͒ of coated and uncoated CaS:Eu particles were performed. While the uncoated phosphor was largely degraded within 30 h of aging, it was observed that a 20 nm thick aluminum oxide coating dramatically increased the resistance of the luminescent material against moisture, showing the conformity of the Al 2 O 3 coating by the ALD process. Upon degradation, CaCO 3 was formed, leading to Eu 3+ emission as observed in cathodoluminescence. Finally, the use of these coated particles as a wavelength conversion material in light-emitting diodes was evaluated.