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Self‐limitation in the surface segregation of Ge atoms in the Si epitaxial overlayers arising from the surface bond geometry on Si(100) during molecular beam epitaxy has been investigated theoretically. It was found that Ge surface segregation is strongly limiting when the Ge concentration exceeds 0.01 monolayer. As a result of this self‐limitation, segregation profiles of Ge in Si overlayers are found to decay nonexponentially in the growth direction with a kink in the profile around 3×1020 cm-3, which is in close agreement with the experimental observation. The kinetic barrier of the Ge surface segregation is estimated to be 1.63±0.1 eV.