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The growing demand for low‐temperature thin‐film encapsulation (TFE) in advanced flexible and wearable organic light‐emitting diodes (OLEDs) has intensified to mitigate thermal issues, which deteriorate the device performance. Herein, Al2O3/TiO2 nanolaminates (A/T NLs)are introduced and fabricated via thermal atomic layer deposition at an exceptionally low temperature of 40 °C, which exhibited enhanced mechanical and environmental robustness. Compared to the single‐layer Al2O3 and TiO2 thin films (0.06% and 0.31%), the A/T NLs with sublayer thickness under 15 nm exhibit dramatic improvement in elongation (0.46–0.53%), attributed to the effective decoupling of critical defects by the Al2O3/TiO2 interfaces. Furthermore, the A/T NLs with 3 nm‐thick‐sublayer demonstrate highly improved water vapor transmission rates of 9.48 × 10−5 g m−2 day−1, making them promising candidates for TFE in wearable OLEDs. Notably, the optimized A/T NL‐encapsulated wearable phosphorescent OLEDs (phOLEDs) exhibit extended lifetimes (LT70), surpassing 200 h in the accelerated environmental conditions (40 °C/90% RH) which is 40 times longer lifetimes compared to the not encapsulated OLEDs. Additionally, the A/T NL‐encapsulated wearable phOLEDs displayed mechanical endurance, enduring 125 h even under the bending strain of 0.4% compared to the Al2O3‐ and TiO2‐encapsulated OLEDs (4 and 18 h). [ABSTRACT FROM AUTHOR]

As transparent, flexible, and wearable organic electronics degrade under normal outdoor environmental conditions (e.g., water vapor, oxygen, and UV light) and extreme environments, including washing or rain, a customized encapsulation technology is required to improve device reliability. Herein, a simple process is presented for fabricating multifunctional hazy substrates (MFHSs) with excellent gas diffusion barrier (GDB), flexibility, UV reflectance, light scattering, and waterproof properties. First, a spiky polyethylene terephthalate (PET) surface is produced with 76.0% optical haze through ion‐beam treatment followed by the formation of a hydrophobic layer to achieve a waterproof effect (contact angle: 153.3°). Then, a multifunctional multibarrier film is fabricated based on a nano‐laminated distributed Bragg reflector and functional polymer on the functional PET substrate to serve as a GDB and UV filter. This multibarrier film has excellent mechanical and chemical stabilities, in addition to having a water vapor transmission rate of 10−6 g m−2 day−1 and UV transmittance of <3%. The so‐fabricated MFHS not only increases the device efficiency by 73% but also enables a highly flexible and environmentally stable organic light–emitting diode. The surface treatment and encapsulation technologies developed in this study are expected to increase the lifetime of organic devices and facilitate high outdoor usability. [ABSTRACT FROM AUTHOR]