This work is focused on the bias stress (BS) effects in Organic Thin-Film Transistors (OTFTs) from poly(2,5-bis(3-alkylthiophen-2-yl)thieno[3,2-b]thiophene) (PBTTT-C14) on both highly-doped Si and glass substrates. While the former had a thermally-grown SiO2 dielectric, the latter demanded an alternative dielectric that should be capable to withstand bottom contact lithography, as well as semiconducting thin-film deposition. In addition, it should represent one more step towards flexible electronics. In order to do that, poly(4-vinylphenol) (PVP) was blended to poly(melamine-co-formaldehyde) methylated (PMF). OTFTs on glass with a cross-linked polymer dielectric had a charge carrier mobility (μ) of 4.0x10-4 cm2/Vs, threshold voltage (VT) of 18 V, current modulation (ION/OFF) higher than 1x102, and subthreshold slope (SS) of -7.7 V/dec. A negative BS shifted VT towards negative values and produced an increase in ION/OFF. A positive BS, on the other hand, produced the opposite effect only for OTFTs on Si. This is believed to be due to a higher trapping at the PVP:PMF interface with PBTTT-C14. Modeling the device current along time by a stretched exponential provided shorter time constants of ca. 105 s and higher exponents of 0.7–0.9 for devices on glass. Due to the presence of increased BS effects, the application of organic TFTs based on PVP:PMF as flexible sensors will require compensating circuits, lower voltages or less measurements in time. Alternatively, BS effects could be reduced by a dielectric surface treatment.