This paper presents the correlation between the functional groups, interfacial microstructure and behavior of load transfer in carbon nanotube (CNT)/epoxy nanocomposites. Nanocomposites consisting of epoxy and CNTs with/without functionalities (amino and epoxide groups) are prepared and characterized to evaluate the CNT-matrix interactions based on strain-sensitive Raman spectroscopy. The results show that nanocomposites filled with functionalized CNTs exhibit a noticeable G'-band shift in tension while those containing pristine CNTs have a marginal shift, suggesting a more efficient load transfer between the epoxy matrix and functionalized CNTs. An interesting observation is that the slope of the G'-band shifts can be either positive or negative, depending on the functional groups on CNTs and the interfacial structures created between the functionalized CNTs and polymer matrix. The mechanisms behind this observation are discussed with reference to fractography and thermo-mechanical properties of nanocomposites. (C) 2012 Elsevier Ltd. All rights reserved.