Abstract Soft pneumatic actuators (SPAs) hold great promise for simple and effective actuation of soft robots. Multi‐degree‐of‐freedom SPAs are highly desired as they enable diverse motion forms and improve possibility for soft robots to navigate challenging environments and perform complex tasks. Herein, this study proposes two novel origami‐based SPAs (O‐SPAs), namely the Flasher origami‐inspired SPA (FO‐SPA) and the Kresling origami‐inspired SPA (KO‐SPA), which are fabricated entirely from soft silicone without any rigid supports. A finite element model is developed to predict the deformation behavior of O‐SPAs and the deformability and dynamic response of O‐SPAs are characterized through performance tests. Simulation experiments are carried out to investigate the impact of different structural parameters on their performance. These O‐SPAs are highly sensitive to low negative pressure, exhibiting 80% of maximum deformation at −4 kPa. Based on the Flasher and Kresling origami pattern, the actuators are capable of generating compound motions including contraction, twisting, and radial motions. These motions can be used as “building blocks” for the rapid reconfiguration of various soft robots. The study has successfully enriched the types of existing SPAs by providing important multiple motions through origami, with great potential to facilitate the rapid and low‐cost design of soft robots.