The effect of ultrasonic melting processing (USP) on three-dimensional (3D) architecture of intermetallic phases and pores in two multicomponent cast Al-5.0Cu-0.6Mn-0.5(1.0)Fe alloys is characterized using conventional microscopy and synchrotron X-ray microtomography. The two alloys are found to contain intermetallic phases such as α-Al15(FeMn)3Cu2, β-Al7Cu2Fe, 2 Al3(FeMn), Al6(FeMn), and Al2Cu that have complex networked morphology in 3D. The application of USP in alloys can obtained refined and equiaxed microstructures. The grain size of 0.5Fe and 1.0Fe alloys is greatly decreased from 16.9 μm, 15.8 μm without USP to 13.3 μm, 12.2 μm with USP, respectively. The results show that USP significantly reduce the volume fraction, grain size, interconnectivity, and equivalent diameter of the intermetallic phases in both alloys. The volume fraction of pores in both alloys is reduced due to the USP degassing effect. The refinement mechanism of USP induced fragmentation of primary and secondary dendrites via acoustic bubbles and acoustic streaming flow were discussed.