The well-known and most widely explored oxide interface is the LaAlO 3 /SrTiO 3 (LAO/STO) heterointerface that was discovered in 2004 to exhibit high-mobility 2DEG, [3] and subsequently shown to reveal fascinating properties such as magnetism, superconductivity, and even coexistence of them. [4][5][6][7] Interestingly, the physical properties of the 2DEG at the LAO/STO interface are controllable through a back gate, [8] a top gate, [9] or an ionic liquid (IL) gate. [10] In particular, the electron mobility can be significantly enhanced by the IL gating, which triggers a switch of the 2DEG between a metallic and an insulating state. [11] To reveal the role of the Ti-ions to the emergent phenomena and obtain higher mobility 2DEG, many attempts to replace STO with other perovskite oxides have been made. [12,13] Among them, KTaO 3 (KTO), a polar and band-insulator (E g ≈ 3.6 eV) oxide, is particularly interesting. [13][14][15][16][17] Similar to STO, a 2DEG is realized at the metallic oxygen-deficient KTO surface [18] or the interface with other materials such as EuO/ KTO, [16] crystalline (c-) LaVO 3 /KTO, [15] amorphous (a-) LAO/ KTO, [15] and c-LaTiO 3 /KTO. [13] As the origin of the electron gas is concerned, similar to STO-based interfaces, the origin of the 2DEG involves electrostatic relaxation and chemical reconstruction driven by the polar discontinuity, [3] interface chemistry, [18][19][20] and oxygen vacancies. [21,22] For a-LAO/KTO interface, the most likely scenario is the oxygen vacancies. In this scenario, the redox reaction at the interface, by oxidizing deposited LAO films and reducing the KTO substrate, accounts for the metallic interface. Furthermore, the gate-tunable 2D superconductivity is exclusively reported for the KTO (111) and (110) based interfaces. [16,23] Intriguingly, the large Rashba coefficient extracted from the spin-charge and chargespin experiments makes KTO-2DEG a potential candidate for spin-orbitronic devices. [23] KTO is a 5d transition metal oxide that exhibits a lighter effective mass of electrons and a stronger spin-orbit coupling (SOC) at its conducting surface/interface than STO-based interfaces. As a result of strong SOC, the low-lying Ta:t 2g band splits at the Γ point and forms the light and heavy bands having the mixed character of d xy , d xz , and d yz orbitals. [18,24,25] Recent Due to the coexistence of many emergent phenomena, including 2D superconductivity and a large Rashba spin-orbit coupling, 5d transition metal oxides-based two-dimensional electron systems (2DESs) have been prospected as one of the potential intrants for modern electronics. However, despite the lighter electron mass, the mobility of carriers, a key requisite for high-performance devices, in 5d-oxides devices remains far behind their 3d-oxides analogs. The carriers' mobility in these oxides is significantly hampered by the inevitable presence of defects. Here, very high mobility (≈22 650 cm 2 V −1 s −1 ) of 5d-2DES confined at the LaAlO 3 /KTaO 3 interface is reported. The high mobility, which ...