This paper presents the design of a pneumatic actuator for a soft ankle-foot orthosis, called the Multi-material Actuator for Variable Stiffness (MAVS). This pneumatic actuator consists of an inflatable soft fabric actuator fixed between two layers of rigid retainer pieces. The MAVS is designed to be integrated with a soft robotic ankle-foot orthosis (SR-AFO) exosuit to aid in supporting the human ankle in the inversion/eversion directions. This design aims to assist individuals affected with chronic ankle instability (CAI) or other impairments to the ankle joint. The MAVS design is made from compliant fabric materials, layered and constrained by thin rigid retainers to prevent volume increase during actuation. The design was optimized to provide the greatest stiffness and least deflection for a beam positioned as a cantilever with a point load. The design of the MAVS took into account passive stiffness of the actuator when combining rigid and compliant materials so that stiffness is maximized when inflated and minimal when passive. An analytic model of the MAVS was created to evaluate the effects in stiffness observed by varying the ratio in length between the rigid pieces and the soft actuator. The results from the analytic model were compared to experimentally obtained results of the MAVS. The MAVS with the greatest stiffness was observed when the gap between the rigid retainers was smallest and the rigid retainer length was smallest. The MAVS design with the highest stiffness at 100 kPa was determined, which required 26.71 ± 0.06 N to deflect the actuator 20 mm, and a resulting stiffness of 1,335.5 N/m and 9.1% margin of error from the model predictions.