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Fermi-level pinning (FLP) effect was widely observed in thin-film transistors(TFTs) with van der Waals (vdW) layered semiconductors (organic ortwo-dimensional) when contact electrodes were thermally evaporated1-3.Intensive investigation was implemented for formation of FLP-free interfacialstates by eliminating chemical disorder and crystal defects arising from metaldeposition4-9. However, technical and principal challenges are still existingtowards high-yield, wafer-scalable and low-cost integration of TFT devices.Herein, we developed a general, scaling-up strategy to fabricate large-scale,high-performance FLP-free organic TFT (OTFT) arrays by using printed vdWcontacts consisting of MXene composite electrodes and 2, 7-dioctyl [1]benzothieno [3, 2-b] [1] benzothiophene (C8BTBT). Room-temperature processesallow for a physically stacked junction without any structural or chemicaldamages. The OTFT arrays can be printed on a large-area silicon wafer orplastic film with 100% yield, exhibit ultrahigh field-effect mobility({\mu}_FE) over 17.0 square centimetres per volt per second (cm2 V-1s-1), highon/off ratio exceeding 108, relatively low contact resistance of 3k ohmmicrometres. The underlying mechanism for the high device performance wasunveiled by Kelvin Probe Force Microscopy (KPFM) combined with theoreticalsimulation. The results indicate that work function (W_F) of the printedelectrodes can be tuned at a wide range of 4.8-5.6 eV, thus significantlylowering the charge-injection barrier at the contact interfaces with idealFLP-free character (the interfacial factor reaches 0.99 \pm 0.02). This studypaves a general strategy for achieving large-scale, high-performance thin-filmelectronics.

High-Yield, Scaling-Up Fabrication of Fermi-Level-Pinning-Free Organic Thin-Film Transistor Arrays with Printed Van der Waals Contacts