Metals and glass are excellent for containing electrolytes and liquids in general, but their rigid mechanics limits their application for mechanically active ionic actuators or flexible/ stretchable electrochemical devices such as batteries and supercapacitors. In this study, we evaluate the performance of spray-coated poly (styrene-block-isobutylene-block-styrene) (SIBS) as a stretchable encapsulant, which suggests that it offers a better combination of compliance and impermeability than any other barrier. We examined the drying time of 360-µm thick encapsulated tri-layer conducting polymer (CP) actuators, comprised of poly(3,4-Ethylenedioxythiophene) (PEDOT) as the CP electrode and an interpenetrated polymer network of polyethylene oxide (PEO) and nitrile butadiene rubber (NBR) as the separator layer, which operates with a 1 M solution of Lithium bis(trifluoromethanesulfonyl)imide (Li+TFSI−) in propylene carbonate (PC). A 100-µm thick SIBS encapsulation layer is anticipated to help these devices to retain 80% of stored PC for more than 1000 times longer compared to when there is no encapsulation (from less than 0.5 days to over 1.5 years). This low permeability combined with the low Young’s modulus of the SIBS film, its biocompatibility, biostability, and FDA approval, as well as ease of fabrication, make this thermoplastic elastomer a promising candidate as an encapsulant for flexible ionic devices such as flexible batteries and supercapacitors, ionic-electrode capacitive sensors, and ionically electroactive actuators. This paves the way for using these devices in implantable and in vivo applications.