New TiO ₂/2D mordenite nanocomposites were synthetized from lamellar mordenite by introduction of titanium tetraetoxide (TEOT) into the interlamellar space with further hydrolysis and calcination. Anatase nanoparticles with an average size of 4 nm form pillars separating mordenite layers, creating mesoporosity. The surface area, pore size distribution, and total pore volume of the nanocomposites depend on the media in which the TEOT hydrolysis occurs. Magic angle spinning nuclear magnetic resonance (MAS NMR) on ¹H, ²³Na, ²⁷Al, and ²⁹Si nuclei was used to study the local structure of synthetized nanocomposites. It was established that in the studied TiO ₂/2D mordenite nanocomposites, the removal of organic cations during preparation results in a partial collapse of the local mordenite structure. ²⁹Si MAS NMR reveals an important contribution from isolated silanol groups (SiO) ₃Si–OH, Q3 sites. The obtained TiO ₂/2D mordenite nanocomposites could be considered as an effective way of immobilization of the TiO ₂ photocatalyst, which creates opportunity for their application for water purification under flow conditions with a high mass transfer.