New materials have come into focus lately for use as dielectric membranes in dielectric elastomer actuators. They are often characterized under differing conditions and their activation behaviour has mostly been investigated on lab-scale samples. This paper aims to compare the activation behaviour of two promising new materials on a macroscale device. The reference material is VHB 4910 (by 3M), which is compared first with a corrugated silicone with silver electrodes (by PolyPower) and second with interpenetrating polymer network-modified acrylic. The permittivity and the electrical break-down strength were measured. Uniaxial tensile and relaxation tests were also carried out. The activation performance was measured with planar actuators in an isotonic and in an agonist–antagonist hinge configuration. The influence of the material properties on the mechanical performance is calculated with simple modelling.