This article describes the synthesis of nanostructured organic/inorganic hybrid materials based on the modification of the titanoniobate oxide KTiNbO5 by N-alkyl amines via an acido-basic reaction. X-ray diffraction and scanning electron microscopy have showed the successful intercalation of the organic molecules between the inorganic layers. The hybrid nanofillers previously obtained have been incorporated in a polyethylene matrix by melt intercalation. The morphology and thermomechanical properties of the nanocomposites have been investigated. It has been revealed that the modification of the oxide improves the dispersion and the exfoliation in the matrix leading to an increase of Young's modulus and of the degradation temperature. The TEM observations coupled with EDS mapping is revealed to be one interesting mean of characterization for this study.