As shown in Fig. 1a, VTES was first hydrolyzed to vinyltetrahydroxysilane (VTHS) in the presence of water and acetic acid, followed by addition of PVP. As soon as VTES is converted to VTHS, sol-gel reactions are considered to begin among VTHS molecules as well as between VTHS and PVP (Si-OH groups in VTHS and C-OH groups in PVP), leading to the precursor sol solutions (VTES- PVP). The precursor solutions were coated on quartz substrates or indium-tin oxide (ITO)-coated glass substrates leading to the VTES-PVP precursor films, which were finally converted to the cross-linked hybrid (X-ASiO-PVPNP) films via thermal curing reaction between double bonds in the silicon atoms. The optical measurement disclosed that the optical absorption spectra (absorption edge) of hybrid (X-ASiO-PVPNP) films were gradually red-shifted as the PVP content increased (see Fig. 1b). However, the optical transparency of films was well maintained even though the film color was changed to slightly yellowish (see the inset photographs in Fig. 1b and Fig. S1). Here we note that the precursor films before thermal cross-linking reactions could be as thick as more than 200 μm by drop-casting from their precursor solutions (see Fig. 1c). The formation of Si-O-C bonds, which are caused by the reaction between the hydroxyl (C-OH) groups in the PVP chains and the silanol (Si-OH) groups in the VTHS domains during sol-gel reactions, was proven by the X-ray photoelectron spectroscopy (XPS) and Fourier Transform-Infrared (FT-IR) spectroscopy measurements (see Fig. 2). As shown in Fig. 1d, the cross-linked hybrid (X-ASiO-PVPNP) films were well coated on the patterned ITO-glass substrates so as to make a gate-insulating memory layer that is placed beneath the P3HT channel layer in the hybrid TOMDs (see the optical microscope images for the channel area in Fig. 1e).