Hydrothermal syntheses of the magadiite, a layered silicate structure, were conducted in the presence of a heteroatom source (SnCl4·5H2O) with the intention of investigating its influence on the resulting material, as well as the possibility of isomorphous replacement of Si by Sn atoms in the above-mentioned structure. For comparison, unmodified magadiite, Al-containing magadiite, and impregnated magadiite were synthesized. The magadiite structure was identified for samples with Sn/Si ratios up to 0.015. Synthetic methods applied to Sn-modified materials were found to be unsuitable for the introduction of Al. The characterization methods used were X-ray diffraction, temperature-programmed reduction, and 29Si magic angle spinning nuclear magnetic resonance and these revealed the substitution of Si by Sn in the silica layers. No additional acid centers on the surfaces of the modified samples were detected, suggesting the presence of the desired four-coordinate Sn in the silica layers.