Protonated forms of layered perovskite-like titanates HLnTiO₄ (Ln = La, Nd), relating to the Ruddlesden-Popper phases, have been used to yield inorganic-organic hybrids with the simplest representatives of amines (methylamine), alcohols (methanol), aminoalcohols (monoethanolamine) as well as n-butylamine. The possibility of the synthesis of the hybrids is studied in a wide range of conditions using both standard laboratory techniques and solvothermal/solvothermal-microwave methods. It is established that only methylamino derivatives may be synthesized in a single-phase form by a direct reaction between protonated titanates and the corresponding organic compound whereas pure n-butylamino, methanolic and monoethanolamino hybrids may be obtained on the basis of methylamino ones. For all the hybrids synthesized structure, quantitative composition, morphology and a type of a bond between inorganic and organic parts are discussed by means of powder XRD, Raman, IR and NMR spectroscopy, STA, elemental CHN analysis and SEM.