Molten carbonate fuel cells (MCFCs) are promising high temperature power generating devices. However, unlike solid oxide fuel cells (SOFCs) they utilize a liquid electrolyte which must be immobilized in a porous matrix. In this paper, a slurry composition for lithium aluminate (gamma-LiAlO2) matrix was developed and green matrices were subsequently formed by the tape casting method. In order to achieve the desired structure of the matrix (pore size, porosity) gamma-LiAlO2 powder was milled in a planetary ball mill for 18 h with a solvent, dispersant and defoamer. After this step, other ingredients were added, including a binder and plasticizer to obtain optimal rheology of the slurry. Cell tests confirmed optimal performance of the matrix compared to the third party reference gamma-LiAlO2 matrices. Burned out matrix was characterized by scanning electron microscopy (SEM) and laser diffraction in order to determine the gamma-LiAlO2 powder particle size and morphology. The results show that high-energy milling enabled a fine pore structure and high specific surface area of the matrix to be obtained in a relatively short time, compared to conventional fabrication routes. The matrix structure obtained within this study is suitable for high performance operation of MCFC. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.