In low-dimensional superconductors, the interplay between quantum confinement and interfacial hybridization effects can reshape Cooper-pair wavefunctions and give rise to unconventional superconducting states. Here we use plasma-free confinement epitaxy assisted by a carbon buffer layer to synthesize a gallium trilayer sandwiched between graphene and a 6H-SiC(0001) substrate. Within this confined gallium layer, we demonstrate interfacial Ising-type superconductivity driven by atomic orbital hybridization. Electrical transport measurements reveal that the in-plane upper critical magnetic field reaches ~21.98 T at T = 400 mK, approximately 3.38 times the Pauli paramagnetic limit. Angle-resolved photoemission spectroscopy measurements, combined with theoretical calculations, confirm the presence of split Fermi surfaces with Ising-type spin textures at the K and K' valleys of the confined gallium layer, originating from strong hybridization with the SiC substrate. This work establishes a strategy for realizing unconventional pairing wavefunctions through the synergistic combination of quantum confinement and interfacial hybridization effects.
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