This paper illustrates the use of a 1 H- 29 Si- 1 H double CP sequence to investigate different organic/SiO 2 interfaces in templated porous silica. The advantage of this sequence is to selectively edit, in a one-dimensional experiment, the protons that are in close proximity with the Si surface sites. In order to maximize the polarization transfer efficiency, some experiments have been recorded at lower temperature (238 K). Examples will concern surfactant/silica interactions in mesostructured silicas and the behavior of benzoic acid and 4-methoxychlorophenol, a common pesticide, encapsulated in mesoporous silica.