Hydrothermal syntheses of a silicate structure comprising a single tetrahedral layer, known as ilerite, were conducted in the presence of tin (SnCl4·5H2O) as a heteroatom. The main aim of the study was to investigate the influence of the above-mentioned compound on the resulting material, as well as the possibility of isomorphous replacement of Si by Sn atoms. For comparison, unmodified ilerite, ilerite impregnated by SnO2, and ilerite synthesized in the presence of Al (aluminum isopropoxide) were also used. The ilerite structure observed was that of Na-ilerite. Syntheses of samples with various Sn/Si ratios (up to the value of 0.01Sn/4Si) and Al/Si ratios (up to the value of 0.005Al/4Si) resulted in a magadiite structure. Synthesis methods applied to Sn-modified materials were found to be unsuitable for the introduction of tetrahedrally substituted Al. The characterization methods used were X-ray diffraction (XRD), temperature-programmed reduction (TPR), and diffuse reflectance infrared fourier transform (DRIFT) spectroscopy. and these indicated the presence of metal oxide species on the surfaces of the crystals, in addition to a small degree of replacement of Si by Sn or Al in the tetrahedral layers.