speed, serious retention degradation, and instability in air still should be overcome for the charge-trap OFETs. [10][11][12] The charge-trap OFET derives from the complementary metal-oxide semiconductor silicon-oxide-nitride-oxide-silicon (SONOS) memory, which is nowadays the most viable solution to replace the current floating gate-based technology and to scale the Flash NAND memories beyond the 16 nm node, [13] although its working mechanism including the carrier transportation in organic semiconductor and the transfer characteristics of OFET is not completely consistent with that of SONOS memory. Recently, much efforts have been made to achieve high performance Si-based chargetrap memory (CTM) devices through matching the energy-band alignments between Si and the charge-trapping dielectric. [14][15][16] It was found that at an applied electric field, the lower difference between the conduction-band minimum of Si and the charge-trapping dielectrics leads to a larger memory window, a higher programming/erasing speed and a better retention characteristics for the CTM devices. So theoretically a nonvolatile charge-trap OFET with matching alignment between the energy band of the charge-trapping dielectric and the corresponding molecular orbitals of organic semiconductor should also get an enhanced performance.ZnTe is an II/VI semiconductor, and the conduction band minimum and the valence band maximum have matching High-performance bottom-gate nonvolatile organic field-effect transistor (OFET) devices based on a special matching energy-band alignment between the organic semiconductor pentacene and the charge-trapping dielectric ZnTe are reported. The lower potential difference between the conduction band minimum of ZnTe and the lowest unoccupied molecular orbital of pentacene with a weak electron conductivity endows the OFET a memory window of 10 V at an applied sweeping gate-voltage of ±15 V, a high I ON /I OFF ratio of more than 10 6 , and good retention with a high I ON /I OFF ratio of 6 × 10 5 after 10 4 s. The large memory window of the OFET is attributed to the unique energy-band alignment of the memory device and the high density of traps in Te-deficient ZnTe film, and the prominent retention is attributed to the deeply trapped electrons in the potential well formed by Al 2 O 3 tunneling and blocking layers.