A solution method of photo-curable and -patternable polymer gate dielectrics was introduced by using blend solutions of poly(4-dimethylsilyl styrene) (PDMSS) and poly(melamine-co-formaldehyde) acrylate (PMFA). The fabrication was optimized to produce a smooth hydrophobic gate dielectric with good insulating and solvent-resistant properties. On the optimized PDMSS/PMFA blend gate dielectric, pentacene could grow into highly ordered structure, showing high electric performances for the resulting OFETs, as well as PTCDI-C13 and TES-ADT.