Nanoscale materials are characterized by a large volume fraction of grain boundaries or interfaces, which can significantly improve the physical and chemical properties of the final product. In order for the properties of nanostructured materials to be obtained, it is necessary that the processing route be carried out correctly. Widely used in ceramic coatings, the phases of the lithium aluminosilicate family, mainly the eucryptite and spodumene-β phase, with low CTE, are used due to the formation of compressive stresses around the grains of the other constituents due to liquid phase sintering. These stresses ensure better properties such as mechanical strength, fracture toughness, and elastic modulus, but producing them on a nanometric scale is challenging. However, their typical production is complex, requiring high process temperatures and long grinding times to obtain micrometric particles. This study aims to synthesize the eucryptite and spodumene-β phases on a nanometer scale and to analyze two different alumina particle sizes to verify which guarantees better efficiency for forming the desired phases. The synthesis of low-CTE lithium aluminium silicate nanoparticles was obtained through a colloidal approach from the heterocoagulation of a lithium source (lithium acetate obtained by the reaction of carbonate with acetic acid), silica (Diameter average: 0,05 µm) , and alumina of two different sizes (Alumina 1: Diameter average of 0,25 µm and Alumina 2: Diameter average of 0,025 µm).  The concentrated suspensions were dried, and the powders were thermally treated at 850 °C to form the crystalline phases projected by the solid-state reaction. The samples were characterized for BET, Thermal Expansion Coefficient and XRD with Rietveld refinement. The coefficient of thermal expansion (CTE) test showed a value of 3.87 x 10-6 °C-1 with Alumina 2 and 1.25 x 10-6 °C-1 with Alumina 1. The XRD test presented mostly spodumene-β and eucryptite phases, in addition to lithium metasilicate and lithium disilicate phases. The Rietveld refinement showed for alumina 1 41.7% spodumene-β (ICSD 26817), 39.20% lithium metasilicate (ICSD 4261), 9.10% lithium disilicate (ICSD 15414) and 10% of Al2O3 (ICSD 026790). With alumina 2, the result was 4.10% spodumene-β (ICSD 26817), 61.5% eucryptite (AMCSD 0376), and 34.4% lithium metasilicate (ICSD 4261).  Powders were synthesized efficiently, which with some adjustments may yield higher levels of β-eucryptite, which might allow us to get higher compressive stress at the interface of the alumina matrix for application in alumina-lithium aluminium silicate composites.