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In present work, a multiphase Ni 3 Al-based intermetallic alloy with complex components of γ'+γ dendrite comprising extremely high volume fraction (81 vol %) of γ′ phase and interdendritic β phase is investigated, the microstructure evolution and phase transformation behavior tailored by different solution cooling rates are studied by applying different cooling methods of water cooling (WC, 138 °C/s), air cooling (AC, 72 °C/s), and furnace cooling (FC, 0.05 °C/s) after solution treatment at 1200 °C for 10 h. Results show that the cubic degree, size and volume fraction of cuboidal primary γ′ as well as size of spherical secondary γ′ particles in the γ'+γ dendrite are improved by decreasing cooling rates, and the average sizes of the primary and secondary γ′ particles are found to meet logarithmic relationships with cooling rates. There are three kinds of precipitates in the interdendritic β phase resulted from different cooling methods, i.e., the rod-like Cr 3 C 2 carbides, the semi-spherical α-Cr particles, and the long acicular γ′ precipitates. The lower cooling rate decreases the number of rod-like Cr 3 C 2 carbides, increases the number and size of the semi-spherical α-Cr particles, and promotes the formation of long acicular γ′ precipitates in the interdendritic β-matrix. The semi-spherical α-Cr particles play the role of pinning dislocations in the β-matrix and have the orientation relationship of [‾110] α-Cr //[‾110] β-matrix. In addition, the precipitation of semi-spherical α-Cr particles in β-matrix is observed to accomplish in two sequential stages and grow in an onion-like ordered way. Stacking faults existed in partial of α-Cr particles due to the nanotwins in β-matrix. Microtwins are observed in the interdendritic β-matrix after water cooling, which have a bimodal configuration of nanotwins at the microtwinning boundaries and interior stacking faults. Besides, γ′-envelope formed between the γ'+γ dendrite and interdendritic β phase dependent on the solution cooling processes. Image 1 • Re-precipitation sizes of primary and secondary γ′ particles have the logarithmic relationship with solution cooling rates. • Microtwins in the β-matrix have a bimodal configuration of nanotwins at their boundary and interior stacking faults. • Precipitation pattern and growth mode of semi-spherical α-Cr particles in β-matrix phase after air cooling. • Precipitation behaviors influenced by solution cooling rates of precipitates in the interdendritic β. [ABSTRACT FROM AUTHOR]