Eu(2-x)Sm(x)Sn2O7 (x = 0, 0.1, 0.5, 1.0, 1.5, and 2.0) solid solutions were successfully synthesized by a simple, mild hydrothermal process. The crystal structure, particle size, and chemical composition of the solid solutions were characterized by X-ray diffraction, transmission electron microscopy, and energy dispersive X-ray spectroscopy. X-ray diffraction patterns and transmission electron microscopy images reveal that all the products were cubic pyrochlore-type Eu(2-x)Sm(x)Sn2O7 nanocrystals with the diameter of approximately 20 nm. Due to efficient energy transfer from Sm3+ to Eu3+, the Eu(2-x)Sm(x)Sn2O7 (x = 0.1, 0.5, 1.0, and 1.5) nanocrystals exhibited strong 5D0 --> 7F1 photoluminescence emission of Eu3+. The dominant 5D0 --> 7F1 transition revealed good monochromaticity and low distortion of the Eu(2-x)Sm(x)Sn2O7 nanophosphors.