One‐dimensional La(OH)3 nanocrystals with multiform morphologies have been successfully synthesized by a facile hydrothermal process without using any surfactant, catalyst, or template. It can be found that the pH values of the initial solutions and the alkaline sources play a crucial role in controlling the morphologies of the products. The possible formation process of the 1D samples was investigated in detail. Furthermore, the as‐prepared Tb3+‐doped La(OH)3 samples show a strong green emission corresponding to 5D4–7F5 transition of the Tb3+ ions under ultraviolet or low‐voltage excitation. The experimental results indicate that the luminescence properties of the as‐obtained phosphors are dependent on their morphologies and sizes. As a result of the unique luminescence properties and controllable morphology and size, these phosphors may find potential applications in fields such as optoelectronic and nanoscale devices or biological technology.(© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2009)