Al2O3 films have long been widely used as inorganic encapsulation or passivation layers. The Al2O3 single layer, however, exhibits not only a relatively low barrier performance but also poor environmental stability under harsh conditions due to its hydrolysis reaction with water vapor. Thus, to further improve its environmental reliability and barrier performance as a gas diffusion barrier (GDB), the GDB should be newly designed by forming a nanolaminate structure with ultra-thin sublayers. In addition, through the use of a multilayer based on nanolaminate/organic layers, the nanolaminate film can be effectively protected by a SiO2-inserted organic layer. In this study, alternately stacked nanolaminate/silane-based organic layers are proposed. The nanolaminate-based multilayer achieved a water vapor transmission rate (WVTR) of 5.94 x 10(-5 )g/m(2)/day under 60 degrees C/90% accelerated conditions. In addition, after a bending test, the nanolaminate-based multilayer showed a WVTR increase by a magnitude of one order under a 0.63% bending strain. The proposed environmentally and mechanically stable hybrid thin-film encapsulation offers a strong potential for the realization of washable, wearable, or flexible displays in the future.