Macrosegregation usually occurs during the vertical centrifugal casting process because of the pressure gradient at different positions during casting. TC4 alloy castings with complicated shapes were produced via a vertical centrifugal casting process, and the effects of the mold rotational speed, centrifugal radius and casting wall thickness on the macrosegregation of the castings were investigated. The results show that macrosegregation in castings produced by the vertical centrifugal casting is greatly enhanced by increasing the rotational speed of the mold. The contents of V and Al in the TC4 castings with smaller centrifugal radii are greater, whereas they are lower in those with larger centrifugal radii, further promoting positive segregation. The distribution of Ti is different from that of V and Al, and it results in negative segregation. The contents of Ti, Al and V at a radius of 71 mm are 88.1 wt.%, 8.1 wt.% and 4.1 wt.%, respectively, and those at a radius of 143 mm are 89.9 wt.%, 7.7 wt.% and 3.6 wt.%, respectively. Element macrosegregation is much more obvious in castings with greater wall thicknesses than in those with thin wall thicknesses because of the lower cooling rates. Overall, the segregation of TC4 alloy castings with complicated shapes is not substantial.