The physical origins of the negative-bias stress (NBS) instability in polymer-based thin-film transistors have been characterized. Through the quantitative analysis by TCAD simulation for the NBS time-dependent experimental results, the threshold voltage (VT)-shift by sub-bandgap density-of-states redistribution forms 70% and 78% for the measured total VT-shift while VT-shift by gate oxide charge trapping only takes 30% and 22% at NBS time of 3000 and 7000 s, respectively. In addition, the increase of source/drain Schottky contact resistance (RSD) is the main reason for NBS-induced on -current (ION) degradation.