Transition-metal-oxide materials and their interfaces have played a dominant role in ionic-based solid state electrochemical devices for energy conversion and storage, for example, as the heart of solid oxide fuel cells, [1] gas sensors, and logic devices of electroresistive memories. [2] Complementing these applications in solid state ionics, in recent years there has been rapid progress in exploring oxide interfaces for electronics. [3][4][5][6][7][8] In particular, the progress in atomic scale control of complex oxide film growth has resulted in the discoveries of a quasi-two-dimensional electron gas (q2DEG) at the heterointerface between two band-gap insulators of perovskite LaAlO 3 (LAO) and SrTiO 3 (STO), [7] and more recently, a 2DEG with extremely high carrier mobilities, exceeding 100,000 cm 2 V -1 s -1 at 2 K, at a epitaxial spinel/perovskite interface between gamma-alumina (γ-Al 2 O 3 , GAO) and STO (GAO/STO). [8] In reminiscent of the realization of high-mobility 2DEGs at epitaxially grown interfaces made of traditional semiconductors, which has led to a wealth of new physical phenomena as well as 2 new electronic and photonic devices over the past few decades, oxide 2DEGs provide opportunities for a new generation of all-oxide electronic devices. [3][4][5][6] On the one hand, like semiconductors, most complex oxides are closely lattice-matched to one another and lead themselves to epitaxial growth. On the other hand, the electrons with partially occupied d-orbitals in transitional metal oxides exhibit stronger correlations to other electrons and the lattice. This can give rise to a variety of extraordinary physical phenomena and functionalities at oxide interfaces well beyond those exhibited by conventional semiconductor interfaces, such as 2DEGs with superconductivity or magnetism. [9,10] Up to date, high mobility oxide 2DEGs are almost exclusively fabricated at temperatures higher than 600 ºC. [3][4][5][6][7][8][9][10][11][12][13] It has become evident that the high-temperature fabrication procedure, firstly, results in strong cation intermixing/diffusion across the interface, [11] which most likely has a deleterious effect on carrier mobilities. For example, the electron mobility of the intensively investigated LAO/STO (deposited at 600-850 ºC) is typically 1000 cm 2 V -1 s -1 at 2 K. [3][4][5][6][7][8][9][10][11][12][13] Similarly, for the high-mobility GAO/STO (deposited at 600 ºC) with film thicker than 3 unit cells (uc), where cation intermixing become unambiguous, the mobility also falls to around 1000 cm 2 V -1 s -1 at 2 K. [8] Secondly, at high temperatures, the oxygen ions in STO can diffuse over many micrometers in minutes. [14] For STObased heterostructures where oxygen vacancies dominate the interface conduction, such as for the GAO/STO heterostructure, [8] the high temperature process can further level out any nanometer-scale steps in the electron concentration profile along lateral directions, although there can be strong spatial confinement vertically. Even for the LAO/STO system, w...