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In situ surface magneto-optical Kerr effect was used in conjunction with scanning tunneling microscopy and low-energy electron diffraction to study the in-plane magnetic anisotropy of ultrathin Fe films on a vicinal Mo(110) substrate. A uniaxial anisotropy with the easy axis of magnetization along the  direction was found for this system down to nearly 2 monolayers coverage, contradicting the results of recent theoretical calculations. The easy axis of a step-induced anisotropy coincides with the surface step edges. © 2004 American Institute of Physics.