Reliable long-term function is crucial for flexible and soft bioelectronics. Mechanical defects and permeation of water molecules across the various device layers are the prime drivers of failure, and particularly in applications requiring continuous contact with biofluids (i.e. for implantable applications). To address demanding needs of miniaturization, mechanical compliance and water impermeability, ultra-thin high-barrier encapsulations are a promising way to improve device reliability. In this work, the encapsulation properties of vapour phase infiltration (VPI) of inorganic Al2O3 layers deposited by atomic layer deposition (ALD), as bilayers with TiO2, onto polyimide and parylene C organic substrates are investigated. The layers are grown in a single reactor and the infiltration is performed in a single process, with a resulting nanometric infiltration depth. Mechanical integrity and hermeticity are characterized through tensile fragmentation tests and accelerated aging tests. Flexible Magnesium sensors monitor water vapor permeability in situ. A remarkable improvement in the crack onset strain (∽2.56 times), interfacial shear strength (∽2.1 times), water vapour transmission rate (∽5.2 times) and lifetime performance (∽7.1 times) is achieved, compared to the non-infiltrated ALD coatings. Pluri-infiltrated multilayers are proposed as alternatives to conventional coatings. This work is envisioned to accelerate research progress on hermetic packaging of flexible bioelectronics.