from the Ti 3d t 2g electrons. Apart from STO, 5d perovskite oxide KTaO 3 (KTO) can also host 2DEG. [19] These 5d 2DEG can be achieved by the Ar + ions irradiating of KTO surface [20] and growing the LaTiO 3 , LAO, or EuO overlayers on top of KTO. [21][22][23] Compared to the 3d STObased 2DEG, the 5d 2DEG exhibit even more remarkable properties. For example, the 2DEG at the interface of LAO/KTO heterostructure exhibits 2D superconductivity with a higher transition temperature, [22] and the 2D magnetic order with high Curie temperature appears at the EuO/KTaO 3 heterointerface. [23] More importantly, different from STO 2DEG, 5d 2DEG expects a stronger spin-orbit coupling. In analogy to LAO/STO, Zhang et al. [24,25] synthesized LAO/KTO heterostructures and discovered high mobility 2DEGs at the interface. They also found that the Rashba effect of the 5d 2DEG can be tuned by back gate voltage and light illumination. However, the LAO overlayer is often found to be amorphous when grown on KTO regardless the deposition temperatures and oxygen pressures during the film growth.For LAO/STO-related heterostructures, it has been discovered that Al-rich capping layer is crucial to ensure a conducting interface. [26,27] Notably, different from perovskite-type conducting oxide interfaces, Chen et al. [28][29][30] prepared the γ-Al 2 O 3 (GAO) film with spinel structure on the STO substrate. A relatively low crystalline temperature (down to room temperature) for GAO is also observed in GAO/STO. [29] The non-isostructural spinel/perovskite interface exists a metallic 2DEG with carrier mobility as high as 100 000 cm 2 V -1 s -1 at 2 K. In contrast to perovskite LAO which shows a large lattice mismatch with KTO (around 4.8%), GAO with spinel structure is a binary insulating metal oxide with bandgap of 8.7 eV, and the lattice constant is a GAO = 0.7911 nm. [31][32][33] This lattice constant matches well with twice of KTO lattice constant (a KTO = 0.3989 nm). Remarkably, such non-isostructural 5d heterostructures of GAO/KTO has never been studied to date. In this letter, we have grown successfully, the epitaxial GAO/KTO heterostructure at different deposition temperatures, and obtained high mobility interfacial 2DEGs with different carrier densities. Furthermore, the carrier density and Rashba spin-orbit coupling (SOC) of the 2DEG are found to be tuned strongly by the laser light. The maximum change of the carrier density is 3 × 10 13 cm -2 , among the largest tunability of complex oxide heterostructures.The 5d 2D electron gas (2DEG) in KTaO 3 -based heterostructures exhibits stronger spin-orbit coupling and higher superconducting transition temperature compared to the 3d SrTiO 3 -based 2DEG, thus attracts much attention recently. However, compared to the intensively investigated isostructural perovskite-type interfaces, the non-isostructural 5d oxide interfaces remain less investigated. Herein, for the first-time, epitaxial spinel/perovskite γ-Al 2 O 3 /KTaO 3 heterointerface is created, at a deposition temperature as low as 300 °C....