A method for the synthesis of the polyaluminosilicates (PAS) with the macromolecules of dendrimer morphology has been developed. A quantum-chemical assessment of thermodynamically possible mechanisms to develop the populations of short-chain aluminosilicates (nuclei of dendrimer macromolecules) has been carried out followed by the domains generation from the dendrimer assemblies capable to contain up to 80 % wt of the dispersed filler particles into their interdomain spaces by means of the GAUSSIAN B3LYP/6-31G (d) software package. A quantitative calculation of the parameters determining the composition of PAS macromolecules and the size of the dendrimer assemblies has been carried out. A method for the synthesis of monomeric precursor-powder has been developed. A new low-temperature ceramic composite material for 3D aerosol printing has been developed on the basis of the PAS and highly dispersed precursor-powder. The processes of 3D aerosol printing of the PAS filled with monomeric precursor-powder have been researched. An optimal method for aerosol generation has been chosen that does not affect the PAS supramolecular structure. The ceramic dielectric layers with high consumer properties have been obtained by means of 3D aerosol printing.