AbstractWe present theoretical studies on the orientation control of micro‐domains in anisotropic laser ceramics. The direction of the crystal axis that is parallel to easy magnetization in each micro‐domain can be aligned along the direction of the applied magnetic field via two steps of fabrication processes. In the first step the alignment is performed during the slip‐casting under the magnetic field, where directions of primary particles are forced to align along the direction of easy magnetization. However, even though rare‐earth trivalent ions doped into primary particles as luminous ions enhance their magnetic moment, the perfect alignment control is not always possible due to Brownian fluctuations by slurry solvent at this stage. The further orientation control can be processed by the preferential grain growth, where an adequate orientation distribution of primary articles in the casted green body is required for the nearly perfect alignment in sintered ceramics. Therefore, it is important for further improvements of anisotropic laser ceramics to find the orientation distribution of primary particles in the slurry, which is determined by the ratio between the anisotropic magnetic potential and the thermal fluctuations. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)