Abstract: Aluminum overlayers on uranium were prepared by sputtering deposition at room temperature in ultra-high vacuum (UHV) chamber. And the process was studied by X-ray photoelectron spectroscopy (XPS). The goal of this work was to study the growth mode of aluminum overlayers as a function of coverage. During deposition, interdiffusion takes place at the Al/U interface, and obvious changes can be observed from the U 4f and Al 2p spectra. The U 4f spectra of Al/U interface show strong correlation satellites at binding energy of 380.4 and 392.7 eV, and plasma loss features at 404.2 eV, respectively. Intensities of the plasma loss features increasing with the coverage of aluminum are corresponding to the enhancement of interdiffusion. Some interactions of aluminum and uranium which yield intemetallic compound UAlx were detected, and this induced 0.2 eV chemical shift to low binding energy to the Al 2p peaks. The result also shows aluminum overlayers grown on uranium follows the volmer-weber mode.