Pentacene thin-film transistor (TFT) memory using poly(2-hydroxyethyl methacrylate) (PHEMA)-based polymer dielectric layers has been developed. The electric performance and memory behaviors of memory TFTs can be significantly improved by using triple polymer dielectric layers consisting of PHEMA/poly(methyl methacrylate) (PMMA)/PHEMA. This can be attributed to the improvement of the channel/dielectric interface. This memory effect is due to the charge storage of the dipolar group or molecules in the dielectric. The devices exhibit a wide memory window (ΔV th, >20 V), switchable channel current, and long retention time.