The performance limits of monolayer arsenic‐phosphorus (AsP) field‐effect transistors (FETs) are explored by first‐principles simulations of ballistic transport in nanoscale devices. The monolayer AsP holds a direct bandgap of 0.92 eV with significantly anisotropic electronic properties. Transfer characteristics of n‐type and p‐type AsP FETs are thoroughly investigated by scaling channel length in the armchair and zigzag direction, respectively. The simulation results indicate that AsP FETs exhibit exceptional device characteristics, such as high on‐state current, short delay time, and low power consumption. Moreover, transfer characteristics demonstrate superior anisotropy on in‐plane electrical transport properties. In particular, in the zigzag direction, even if the channel length is scaled down to 4 nm, the device performance still can satisfy the International Technology Roadmap for Semiconductors high‐performance requirement. Finally, through benchmarking energy‐delay product against other typical 2D FETs, AsP FETs are revealed to be strongly competitive 2D FETs.

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2D puckered materials similar to black phosphorene (BP) have tunable electronic structures, high mobility, and anisotropy, and are expected to become possible candidate channels for post‐silicon field‐effect transistors (FETs). Herein, monolayer α‐CS with puckered structure is evaluated as a promising channel material for sub‐5 nm FETs by using first principle quantum transport simulation. Monolayer α‐CS FETs can satisfy the requirements of the International Technology Roadmap for Semiconductors (ITRS) for high‐performance (HP) and low‐power (LP) applications. The on‐state current can reach 3700 µA µm−1 for HP FET at 5 nm channel length and the on‐off ratio of LP FET is exceeding 107, both superior to those of other 2D channels like BP and InSe. The results suggest that α‐CS as a competitive channel material opens a new avenue for the future electronic technology in the upcoming Internet of Things.