We are investigating the use of dielectric elastomers (DE) to realize origami-inspired folding and unfolding of structures. DEs are compliant materials where the coupled electro-mechanical actuation takes advantage of the low modulus and high breakdown strength of the elastomer. Until recently, pre-straining of relatively thick DE materials was necessary in order to achieve the high electric fields required to trigger electrostatic actuation. However, the current availability of thinner DE materials (ex: VHB 9469PC-130μm, VHB 9473 PC -260 μm) has enabled their actuation at achievable electric fields without the need to pre-strain. In this work, an exhaustive study on the fundamentals of DE actuation is done by exploring thickness actuation mechanism and studying the change in dielectric permittivity; we also take advantage of the thin DEs to build actuators with very large bending angles. In particular, we relate the electrostatically-induced thickness contraction in a DE monomorph to the resulting bending once an inactive substrate is added. Both statically and dynamically induced electromechanical thickness strains are measured, and the experimental data is used as an input to a bender model to predict and optimize bending response; variables such as type of inactive material, number of DE layers, and type of electrodes are examined. We will also experimentally track the changes in the dielectric constant as a function of strain, electrode type, and applied electric field; the measured behavior will be used to model thickness and bending actuation. These fundamental studies are necessary to determine ability and limitation of DE materials in a bender configuration. Finally, bending of the DE actuator is transformed into folding by a novel geometric approach, where different shaped notches are introduced in the inactive substrate. The folding configuration is a step towards realizing active origami structure.