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The multi-frequency capacitance-voltage (C-V) spectroscopy is proposed for extracting the sub-bandgap density-of-states (DOS) of polymer semiconductors and demonstrated in three different thiophene-based organic thin-film transistors including poly(3-hexylthiophene), poly(3,3 000-didodecylquaterthiophene), and poly(didodecylquaterthiophene-alt-didodecylbithiazole). The density of exponential tail and exponential deep states are extracted to be in the range of 3.0 Â 10 18 $ 1.5 Â 10 19 cm À3 eV À1 and 3.0 Â 10 16 $ 3.0 Â 10 17 cm À3 eV À1 , respectively. The extracted DOS correspond to the polymer semiconductor-dependence of the measured crystallinity and mobility. In addition, the extracted DOS values are verified by comparing the measured I-V characteristics with the simulated results through a technology computer-aided design tool.