Convex surface modification of carbon nanofibers (CNFs) through covalent functionalization plays a pivotal role in the world of polymeric nanocomposites. The free radical 'grafting from' technique was successfully applied for the first time for synthesis of 2-methyl oxazoline-grafted carbon nanofibers (Oxa-g-CNF). The resulting Oxa-g-CNF was characterized by infrared spectroscopy, thermogravimetric analysis and wide angle X-ray studies. Moreover, the synthesised Oxa-g-CNF was utilized for the preparation of acrylic elastomer-based nanocomposite targeted for model elastomeric actuators by solution casting technique. The nanocomposite showed excellent increase in relative permittivity proportional to actuation pressure, when compared with pristine acrylic elastomer and commercial materials. The improvement of properties was ascribed to excellent interaction between modified carbon nanofibers and polar group of acrylic elastomer. This technique adopted promises to open up a new avenue for facile preparation of acrylic elastomeric actuators.