A general nonaqueous route has been applied for the preparation of rare-earth ordered nanocrystalline hybridstructures. In a simple one-pot reaction process, Y
3+ and Gd
3+ isopropoxides were reacted in an autoclavewith 4-biphenylmethanol at 275
C. This approach leads to crystalline rare-earth oxide thin layers (~0.6 nm)regularly separated from each other by organic layers of biphenolate molecules. The optical properties ofthese hybrid materials doped with Eu
3+ and Nd
3+, which are optical active lanthanides ions emitting in thered and near infrared, respectively, are presented. They show significant advantages compared to standardphosphors, such as higher radiance and
luminance va
lues, the possibility to tune the emission chromaticityby varying the excitation wavelength, and a much larger excitation range (250-350 nm and 300-500 nm forthe Eu
3+ and Nd
3+ doped nanohybrids, respectively) shifted toward the red.