Previously unknown in the literature, complexes of hexamethylenetetramine (HMTA) with tungsten silicates of the composition Rb5[SiW11O39Fe(HMTA)]?20H2O, Cs5[SiW11O39Fe(HMTA)]?6H2O, Rb6[SiW11O39Zn(HMTA)]?12H2O, Cs6[SiW11O39Zn(HMTA)]?10H2O with the Keggin anion structure were synthesized and studied by electron and IR spectroscopy, nuclear magnetic resonance, thermal and X-ray phase analysis. The electronic absorption spectra of the HMTA complexes with tungsten silicatoferrates in the region of 270…600 nm indicate an octahedral environment of iron (III) atoms, and the shift of the absorption maximum of 290 nm for Rb5[SiW11O39Fe(H2O)]?10H2O to 310 nm for Rb5[SiW11O39Fe(HMTA)] indicates a change in the ligands in the immediate environment of iron atoms and the formation of HMTA complexes with tungsten silicate. This is also evidenced by the results of nuclear magnetic resonance of solutions of the synthesized zinc-containing compounds in D2O: the chemical shift of the 1H protons of the CH2 methylene groups in HMTA is 4.56 ppm, in the Rb6[SiW11O39Zn(HMTA)]?12H2O complex – 4.64 ppm; for the 13C carbon atoms in HMTA, the chemical shift is 71.1 ppm, and in the Rb6[SiW11O39Zn(HMTA)]?12H2O complex – 71.2 ppm. According to thermal analysis (TA), differential scanning calorimetry (DSC) and X-ray phase analysis, the products of thermolysis of the synthesized compounds at 650? are phases with the structure of pyrochlore and hexagonal tungsten bronzes. The catalytic properties of Rb5[SiW11O39Fe(HMTA)]?20H2O were studied in the production of carbon nanomaterials. A hybrid carbon-mineral material, nanocarbon (WOX), was obtained. It was characterized by X-ray diffraction analysis and electron microscopy. It exhibits high electrical conductivity and chemical resistance to concentrated acid solutions. The results of this study may be useful for the low-temperature synthesis of compounds with a pyrochlore structure, hexagonal tungsten bronze, and hybrid carbon-mineral nanostructures.