In conclusion, novel polymer nanodot-embedded alkyl silicon oxide hybrids, X-ASiO-PVPNP, were successfully prepared via sol-gel and chemical cross-linking reactions. The surface of PVP nanodots (PVPNP = 1~3 nm from HRTEM) with a particular lattice nanostructure (inter-lattice spacing = 0.15~0.2 nm) was found to make covalent bonds with the cross-linked alkyl silicon oxide (X-ASiO), which might be a driving force to generate such a small PVPNP leading to high thermal stability. The hybrid transistor-type organic memory devices (TOMDs) with the X-ASiO-PVPNP layers exhibited stable operation at 150 °C during >4750 WRER cycles, which is the first record for TOMDs tested at a high temperature. Therefore, the present X-ASiO-PVPNP hybrid materials are expected to be a landmarking milestone for achieving durable organic memory devices with excellent operation stability at high temperatures. In addition, the synthesis protocols of X-ASiO-PVPNP materials can be useful to invent super-strong flexible transparent substrates and thermo-resistive functional coatings for flexible electronic devices because the embedded (hybridized) polymer nanodots are expected to play a critical role in compensating mechanical stresses together with high thermal stability by the X-ASiO domains.