Soft, physically crosslinking, block copolymer elastomers were filled with surface-treated nanoparticles, in order to evaluate the possibility for improvement of their properties when used as soft dielectric actuators. The nanoparticles led to improvements in dielectric properties, however they also reinforced the elastomer matrix. Comparing dielectric spectra of composites with untreated and surface-treated particles showed a measurable influence of the surface on the dielectric loss behaviour for high filler amounts, strongly indicating an improved host–guest interaction for the surface-treated particles. Breakdown strength was measured using a test bench and was found to be in good agreement with the results from the actuation measurements. Actuation responses predicted by a model for prestrained actuators agreed well with measurements up to a filler amount of 20%_vol. Strong improvements in actuation behaviour were observed, with an optimum near 15%_volnanoparticles, corresponding to a reduction in electrical field of 27% for identical actuation strains. The use of physically crosslinking elastomer ensured the mechanical properties of the matrix elastomer were unchanged by nanoparticles effecting the crosslinking reaction, contrary to similar experiments performed with chemically crosslinking elastomers. This allows for a firm conclusion about the positive effects of surface-treated nanoparticles on actuation behavior.