A glow like atmospheric pressure dielectric barrier discharge in a roll‐to‐roll setup was used to synthesize 90 nm silica‐like bilayer encapsulation films composed of a 30 nm dense “barrier layer” and a comparatively less dense 60 nm “buffer layer” onto a polyethylene 2,6 naphthalate substrate by means of plasma enhanced chemical vapor deposition. Tetraethyl orthosilicate was used as the precursor gas, together with a mixture of nitrogen, oxygen, and argon. The microstructure, chemical composition, morphology, and permeation properties of the films were studied as a function of the specific energy delivered per precursor molecule, and oxygen concentration in the gas mixture, during the deposition of the barrier layer. The presence of the buffer layer within the bilayer architecture critically enhanced the encapsulation performance of the bilayer films, and this in conjunction with increasing the specific energy delivered per precursor molecule during the barrier layer deposition to a value of 20 keV, enabled an effective water vapor transmission rate as low as 6.9 × 10−4 g m−2 d−1 (at 40 °C, 90% relative humidity (RH)) to be achieved. Furthermore, the bilayer film structure has given rise to a remarkable 50% reduction in deposition energy consumption per barrier area with respect to single layer silica‐like films of equivalent encapsulation performance and thickness.