Flexible devices often need a protective coating when operating in harmful environments, ranging from mild ambient conditions to a biologically active environment of the human body. The flexibility poses a problem for traditional encapsulation solutions, as those make the device bulky and limit functionality by applying an external casing. Alternatively, fully conformal encapsulation of a device of arbitrary shape can be realized with thin film encapsulation (TFE) without altering device dimensions. Yet TFE is susceptible to fail under mechanical stresses, especially when a hard ceramic coating is applied on a polymer. Reliability of TFE can be enhanced by altering the elasticity of the hard and brittle thin films, by adding softer layers in between sample and barrier. In this work, molecular layer deposited (MLD) metal‐linked trioxysilylheptanoate (M‐TOSH) films are studied for coating of large devices to conformally and uniformly tune the interface between polymer and atomic layer deposited protective film. The results show that M‐TOSH process scales to large chambers, parameter optimization leads to superior film quality and lowers elastic modulus. Conformality, tested with home‐built macroscopic test device, found the process suitable for 3D parts. Final testing revealed that 10 cycles of MLD‐interlayer doubled the crack‐onset‐strain from 0.26% to 0.51%.This article is protected by copyright. All rights reserved.