Fig. S1 PMMA transfer method

Fig. 1 Characterization of MoTe2 film and electrical measurement of Au/Ti/MoTe2/Au/Ti device (a) Photo of the centimeter-scale MoTe2 film; (b) Raman spectrum of the MoTe2 film; (c) Optical image of the prepared memristive devices with the structure of Au/Ti/MoTe2/Au/Ti; (d) Optical image of a 3×3 memristor array

Fig. S2 XRD pattern of the MoTe2 film

Fig. S3 Fabrication process of the Au/Ti/MoTe2/Au/Ti device

Fig. S4 AFM image (a) of 3×3 memristor array, and the height profile (b) along the horizontal line and the vertical line

Fig. S5 Electroforming process of the device

Fig. 2 Stable bipolar resistive switching behavior and retention characteristics of the MoTe2 device (a) 20 cycles of I-V curves with a compliance current of 3 mA; (b) Retention characteristics of the HRS and the LRS read at 0.1 V

Fig. 3 Fast switching and good endurance of the MoTe2 device (a) SET speed under the pulse with the amplitude 1.3 V; (b) RESET speed of the MoTe2 device under the pulse with the amplitude of -1.0 V; (c) Over 2000 switching cycles obtained by applying SET pulse of 1.7 V/700 ns and RESET pulse of -1.2 V/7 μs Colorful figures are available on website

Fig. S6 I-V curves of 24 Au/Ti/MoTe2/Au/Ti devices All devices show stable resistive switching with low cycle-to-cycle and device-to-device variability

Fig. 4 Cumulative distribution of (a) VSET and (b) VRESET of 24 devices

Fig. S7 Cumulative distribution of device (a) HRS and (b) LRS of 24 devices

Fig. S8 Estimation of the array size for the prepared CVD-MoTe2 device (a) Sneak current path at read in a square crossbar array where all bits except the selected one are at LRS, and the equivalent circuit can be represented by three resistors (region 1, region 2 and region 3); (b) Dependence of the read margin on the crossbar line number for both 1R and 1T1R schemes

Fig. S9 I-V characteristics of the Pt/TaOx/TiO2/TaOx/Pt selector[4]

Fig. 5 Stable resistive switching of the MoTe2 array device after electroforming process (a) Electroforming process of the MoTe2 array device; (b) 20 cycles I-V curves of the MoTe2 array device with a compliance current of 5 Ma

Fig. S10 I-V curves of 9 devices in 3×3 array

Fig. S11 Long-term potentiation and depression of the device using 50 potentiation (1 V, 500 ns) and depression (-1 V, 5 µs) presynaptic pulses

Fig. 6 Potentiation and depression processes of the present device Circles are experimental results, red lines are fitting results with a phenomenological model $G=a+c{{e}^{-\beta N}}$

Fig. 7 Recognition accuracy for small and large handwritten digit images with experimental devices and ideal numeric Colorful figures are available on website

Fig. 8 Mechanism analysis of the memristive behavior in the MoTe2 device (a) I-V characteristics at HRS under different temperatures, with current increasing as the temperature increases Fitted data using the Schottky emission model for HRS is shown in the inset; (b) I-V characteristics at LRS at different temperatures, with current decreasing as the temperature increase, indicating a metallic characteristic