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We have combined x-ray diffraction studies with first-principles calculations to study the interplay between segregation and ordering at the (110) surface of Ni90Al10. We find a L1(2)-ordered monolayer at the surface. The observed ordering as well as recently reported Al segregation at the surface are explained in a consistent picture. A delicate competition between the tendency for Al segregation and ordering in the Ni-Al system induced by the symmetry break at the surface stabilizes a long-range ordered surface in the entire concentration range c(Ni) > 0.75,