Devices based on organic semiconductors (OSCs) play a significant role in modern life. In general, OSC materials have two main classes, namely π-conjugated small molecules and polymers. [1,2] Based on the majority of the donating and accepting systems in the material, OSCs are classified as n-and p-types. In the frame of reference for electronic transport, n-type OSCs are formed from electron-accepting systems, while p-type OSCs are formed from electron-donating systems. Both classes have received considerable attention from academia and industry owing to their excellent properties, such as low-temperature processing, light weight, low cost, good mechanical properties, flexibility, and large-area capability. Numerous organic microelectronic and optoelectronic devices are based on these two classes of OSCs, for example, organic memories, organic sensors, light-emitting devices, solar cells, and thin-film transistors. Devices based on n-and/or p-type OSC materials are still a subject of intensive efforts by numerous researchers. Organic thin-film transistors (OTFTs) are considered one of the most expeditiously developed technologies, as they are based on organic structures and present an immense potential to ultimately compete with their silicon counterparts. [1,3,[9][10][11] Fundamentally, the organic conductive channels in OTFTs can be p-type or n-type. In addition, there is another type of organic conductive channel based on OSCs, namely, the ambipolar OSC, which can transport both types of charges (via electron transport and hole transport) simultaneously. [1,22,23] To date, many superior OTFTs based on p-type OSCs have been developed. However, OTFTs possessing n-type characteristics have not been developed. One of the most important reasons for this is the instability of n-type organic structures in ambient atmosphere, wherein oxygen and water molecules are abundant and can act as electron traps. [22,23] Moreover, the barrier of injection between the level of the lowest unoccupied molecular orbital (LUMO) of the n-type structures and the work function of most types of electrodes make injection more difficult and consequently, reduce the density of electrons that can participate in the transport; this results in a poor performance of the n-type OTFT devices. [22,23] Despite these limitations, air-stable highefficiency n-channel OSCs continue to be improved because they remain indispensable and vital from a practical point of view for many organic device applications, such as complementary circuits, p-n junctions, and ambipolar transistors. [4][5][6][7][8][9]22,23] Thus, it is essential to investigate and enhance the efficiency of the n-type transistors. This inevitably requires an understanding of the mechanisms of electrical conduction and stability. To this end, several n-type OSCs, such as the family of perylene tetracarboxylic diimide (PTCDI) as well as fullerenes, and their derivatives, have been utilized in OTFTs with n-channels as active layers. [24][25][26][27][28][29] Interestingly, N,N 0 -dioctyl-3,...