New hybrid organic-inorganic derivatives HLnTiO₄ · CH₃NH₂ (Ln = La and Nd) are obtained via the intercalation of methylamine into the interlayer space of protonated layered perovskite-like titanates HLnTiO₄. The existence of three stable methylamine derivatives, namely, α-, β-, and γ-forms, is found for each of the titanates. The thermal stability of the obtained intercalation products is studied and their structural parameters are determined.