Using synchrotron X-ray diffraction, tomography and machine-learning enabled phase segmentation strategy, we have studied under operando conditions the nucleation, co-growth and dynamic interplays among the dendritic and multiple intermetallic phases of a typical recycled Al alloy (Al5Cu1.5Fe1Si, wt.%) in solidification with and without ultrasound. The research has revealed and elucidated the underlying mechanisms that drive the formation of the very complex and convoluted Fe-rich phases with rhombic dodecahedron and 3D skeleton networks (the so-called Chinese-script type morphology). Through statistical microstructural analyses and numerical modelling of the ultrasound melt processing, the research has demonstrated that a short period of ultrasound processing of just 7 s in the liquid state is able to reduce the average size of the α-Al dendrites and the Fe-containing intermetallic phases by ∼5 times compared to the cases without ultrasound. For the first time, this work has revealed fully the nucleation and growth dynamics of the convoluted morphology of the Fe-containing intermetallic phases in 4D domain. The research has also demonstrated clearly the beneficial effects of applying ultrasound to control the Fe phases' morphology in recycled Al alloys and it is one of the most effective and green processing strategies.