In the present work, the use of microsecond and nanosecond laser pulses to alloy copper in aluminum is presented. In the first run, high purity (99.999%) copper thin film was thermally evaporated over (99.9%) purity, 300 μm aluminum sheet. Thereafter, surface alloying was performed using (1–3) 500 μs, (0.1–1.5) Joule Nd: YAG laser pulses; operating at 1060 nm wavelength. Hard homogeneous alloyed zone was obtained at depths between 60 and 110 μm below the surface. In the second run, 9 ns laser pulses from Q-switched Nd: YAG laser operating at 1060 nm was employed to melt/alloy Al-Cu sheets. The resulted alloyed depth, after using 20 laser pulses, was 199.22 μm for Al over Cu samples and 419.61 μm for Cu over Al samples. X-ray diffraction and fluorescence analysis revealed the formation of Cu2Al2, CuAl2 and δ- Al4Cu9 phases with percentage depended on laser energy and copper layer thicknesses.