Low temperature, solution-processed metal oxide thin film transistors (MEOTFTs) have been widely investigated for application in low-cost, transparent, and flexible electronics. To enlarge the application area, solution-processed gate insulators (GI) have been investigated in recent years. We investigated the effects of the organic/inorganic bi-layer GI to ZnO thin film transistors (TFTs). PVP, YO(x) nanoparticle composite, and polysilazane bi-layer showed low leakage current (-10(-8) A/cm2 in 2 MV), which are applicable in low temperature processed MEOTFTs. Polysilazane was used as an interlayer between ZnO and PVP, YO(x) nanoparticle composite as a good charge transport interface with ZnO. By applying the PVP, YO(x), nanoparticle composite/polysilazane bi-layer structure to ZnO TFTs, we successfully suppressed the off current (I(off)) to -10(-11) and fabricated good MEOTFTs in 180 degrees C.