Functionalization of CNFs with silane coupling agents (SCAs) has been studied in this work. APS silane has been used in order to study the influence of temperature and reaction time on the silanization process. Thermal analysis and surface area measurements have revealed that reaction times higher than 1 min. and temperature reaction higher than 25°C do not increase the amount of adsorbed silane on CNFs surface. Silanization process carried with different SCAs (APS, AMO, DMO and GMO) has allowed the study of the concentration and silane structure influence. It has been observed that differences in SCA adsorption are related to the silane structure. Aminosilanes APS and AMO show a very similar behaviour because they have the same functional group. However, the diaminosilane DMO shows lower interaction with CNFs surface due to the length of the diamine chain, that avoid further silane adsorption on the coated CNFs surface. The epoxysilane GMO shows a similar behaviour to other SCAs at low concentrations, while for high silane concentrations epoxysilane GMO forms multilayers.