Atomically thin layers of van der Waals (vdW) crystals offer an ideal material platform to realize tunnel field-effect transistors (TFETs) that exploit the tunneling of charge carriers across the forbidden gap of a vdW heterojunction. This type of device requires a precise energy band alignment of the different layers of the junction to optimize the tunnel current. Among 2D vdW materials, black phosphorus (BP) and indium selenide (InSe) have a Brillouin zone-centered conduction and valence bands, and a type II band offset, both ideally suited for band-to-band tunneling. TFETs based on BP/InSe heterojunctions with diverse electrical transport characteristics are demonstrated: forward rectifying, Zener tunneling, and backward rectifying characteristics are realized in BP/InSe junctions with different thickness of the BP layer or by electrostatic gating of the junction. Electrostatic gating yields a large on/off current ratio of up to 10 8 and negative differential resistance at low applied voltages (V ≈ 0.2 V). These findings illustrate versatile functionalities of TFETs based on BP and InSe, offering opportunities for applications of these 2D materials beyond the device architectures reported in the current literature.challenges require a shift from traditional approaches toward transformative material systems and integration technologies. [1,2] Atomically thin layers of van der Waals (vdW) crystals and their heterostructures, [3][4][5] generally referred to as 2D materials, offer opportunities to study and exploit quantum phenomena for a wide range of applications. [6][7][8][9][10] These crystals have strong covalent atomic bonding in the 2D planes and weak vdW interaction between the layers, which enable the fabrication of stable thin films down to the atomic monolayer thickness and stack them into multilayered heterostructures. [11][12][13] The science of these 2D systems is developing rapidly with important technological breakthroughs emerging from recent studies.Among the extended family of 2D systems, the metal chalcogenide indium selenide (InSe) [14][15][16][17][18] and the elemental compound black phosphorous (BP) [19][20][21][22][23][24] have received increasing attention. These two semiconductors have electronic properties distinct from those of other 2D materials, such as transition metal dichalcogenides (TMDCs), including a higher electron mobility beneficial for field-effect transistors