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In present work, the unique envelope structure (about 1.1 μm in width, and ~3 vol%) in an as-cast multiphase Ni 3 Al-based intermetallic alloy was characterized in detail, its formation mechanism during solidification and widening behavior during long-term aging process were analyzed, and relevant effects on creep behaviors of this Ni 3 Al-based intermetallic alloy under 800 oC/220 MPa were evaluated. Results show that the envelope structure located between the γ'+γ dendrite and interdendritic β phase is γ′-Ni 3 Al phase with ordered face-centered L1 2 structure, which plays a vital role in adjoining the heteroid γ'+γ dendrite/interdendritic β phases. The γ′-envelope possesses a coherent orientation relationship of [101] γ'-envelope //[01‾1] dendritic-γ with the dendritic-γ phase (face-centered A1 structure) due to their similar face-centered lattice type, while there exists a semi-coherent transition region between the γ′-envelope (face-centered L1 2 structure) and interdendritic β phase (body-centered B2 structure) to accommodate their relative lattice mismatching. The formation of γ′-envelope during solidification process is induced by nickel enrichment in the residual liquidoid after interdendritic β phase, and its widening during long-term aging at 800 oC is mainly controlled by the diffusion of Ni, Al, Hf and Mo atoms at the interfaces between γ'+γ dendrite/γ′-envelope/interdendritic β phase under thermal activations, involving the relevant phase transformation of β (NiAl) + γ (Ni) → γ' (Ni 3 Al). The widening of γ′-envelope resulted in a decrease of interdendritic β phase and an increase of γ′ phase in volume fraction, benefited in the improved creep rupture life and reduced steady-state creep rate. However, the γ′-envelope widening also plays a positive role in crack initiation during creep deformation, since besides the GBs and the semi-coherent interfaces of the γ′-envelope/interdendritic β, cracks are also found to initiate near the Cr 23 C 6 carbides surrounded by the widened γ′-envelope. [ABSTRACT FROM AUTHOR]