Raman spectroscopy investigations on nanocomposites obtained by dispersing halloysite within isotactic polypropylene are reported. A detailed analysis of the modifications of the regularity band associated to the polymeric matrix is presented. The Raman lines assigned to the polymeric matrix are broadened and weakened as the loading with halloysite is increased. The analysis of Raman lines indicates that the polymeric matrix becomes less crystalline upon the loading with halloysite and that the nanofiller is experiencing a weak dehydration upon dispersion within the polymeric matrix, probably due to the related thermal processing used to achieve the dispersion of halloysite.