robustness to mechanical stress. The combination of these two properties is typically found in inorganic materials such as metals and metal oxides, therefore inorganic materials which are able to selfrecover are in high demand. [3] Examples of self-healing materials for applications in electronics and related fields are scarce. The few existing ones describe materials that can restore their crack-degraded conductivity, [4] including semiconducting polymers, [5] conductive polymer networks, [6,7] microchannels, and microcapsules filled with Ga-based liquid metal alloys, [8,9] or metal-containing solutions, [10] and ionic hydrogels. [11,12] Further progress remains challenging, primarily because of the lack of feasible healing agents and suitable ways to supply them to the damaged site. In theory, the most logical way to construct self-healing materials is by the entrapment of reactive precursors within the bulk material which reacts only upon exposure to air, for example at a damaged site. Unfortunately, this is a complex and potentially dangerous approach due to the reactivity of the applied chemicals. [10] We aim to widen the pool of self-healing materials from soft matter toward metal oxides (MeOs), including the highly demanded transparent conductive oxides (TCOs). MeOs are typically very inert in ambient conditions. Healing cracks in MeOs by recrystallization would require considerable energy investment. If a device contains polymers, for example as a substrate in the case of flexible electronics, such an energy input will be incompatible with the thermal range of the polymers and is therefore not applicable. Self-healing of inorganic materials and structures could alternatively be realized by loading a polymeric substrate with inorganic nanoparticles (NPs) and enabling their mobility inside the substrate. The spatial distribution of NPs can be tuned by harnessing both enthalpy and entropy. [13][14][15][16] In suitable material systems, the NPs can migrate to new damage-induced interfaces, agglomerating and thereby performing self-healing events. [17] However, a polymer coating on inorganic NPs was required in that work, which shielded the NPs and therefore affected their functional properties. [17] An entropy-driven NP reorganization, as described in this work, suggests a promising and safe alternative pathway to allow the healing of metal oxides. As a first step, a system with MeO nanoparticles, well-dispersed inside a preferably polymeric host matrix, is needed. This can be obtained by vapor phase infiltration (VPI) of a polymer with inorganic materials. [18][19][20] The approach will yield a hybrid or nanocomposite polymerinorganic material with an inorganic thin film coating of the same or another MeO, depending on the process setup. [21] This Enabling self-healing of materials is crucially important for saving resources and energy in numerous emerging applications. While strategies for the selfhealing of polymers are advanced, mechanisms for semiconducting inorganic materials are scarce due to the lack ...