Dynamical manipulation of oxygen ion (O 2− ) at metal/oxide heterointerfaces is widely demonstrated to tailor numerous physical and chemical properties and facilitate creating novel functionalities significantly. The traditional works mainly focus on electric control of O 2− dynamical behavior and related interface characteristics. Here, an alternative strategy is reported to modulate O 2− transport and interfacial magnetism via a significant strain induced by shape memory effect, which is different from the conventional magnetoelastic coupling mechanism. By driving the martensite to austenite transition in TiNi(Nb) shape memory alloy substrates, a significant and tunable strain is exerted on Pt/Co/MgO heterostructure, which promotes interfacial O 2− migration in a nonvolatile manner. The O 2− migration induces an orbital reconstruction of Co to tune the orbital magnetism noticeably, which strengthens the interfacial magnetic anisotropy energy by two times to a striking value of 0.95 erg cm −2 . Besides, the overall magnetic anisotropy is broadly tunable from in-plane to perpendicular direction by an elaborate strain engineering with changing Co thickness. This work develops a nonelectrical oxygen manipulation for tailoring ion-controlled interfacial properties universally and also clarifies the magnetoionic coupling origin for enriching the oxygen-related orbital physics and functional device applications. and interfacial performance can advance the metal/oxide bilayer applications to functional devices. Of particular recent interest in the information storage and sensing fields are the ferromagnetic metal (FM)/metal-oxide (MO) bilayers with a strong perpendicular magnetic anisotropy (PMA), such as CoFeB/MgO and Co/AlO x , which are the core elements of low energyconsumption spintronic devices, such as magnetic tunneling junction, magnetic random access memories, and racetrack memorizers. [19][20][21][22][23] The PMA of FM/MO bilayers mainly derives from the interfacial FM 3d-O 2p orbital hybridization that is sensitive to the interfacial oxygen environment. [1][2][3][4][5][6] Therefore, extensive works were carried out to tailor the interfacial magnetism by controlling O 2− transport especially using an electric field. [5,7,[24][25][26][27][28] The electric field can drive O 2migration to change oxidation state of FM layer, which can regulate the magnetic anisotropy energy (MAE), [7,[24][25][26][27] which paves a feasible way for markedly reducing the switching energy in solid-state spintronic devices. However, to apply an effective electric field, a thick MO layer of tens of nanometers is required to ensure its good insulativity, which may restrict the application on devices with thin MO layers. Moreover, besides the dynamical O 2− migration, the electric field also causes a static charge accumulation to affect the MAE of FM layer concurrently, [29][30][31][32][33] which makes the in-depth magnetoionic coupling origin still ambiguous. Thus, developing a Interfacial Magnetic Anisotropy