Laser-induced alloying effects on the composition and structure of different Ni/Ti multilayer structures were studied. Thin films composed of one, five, and ten (Ni/Ti) bilayers were deposited by DC ion sputtering on (100) Si wafers. Laser irradiations were performed by 150ps pulses of a Nd:YAG laser operating at 1064nm. The samples were characterized by Rutherford backscattering spectrometry (RBS), Auger electron spectroscopy (AES), X-ray diffraction (XRD), atomic force microscopy (AFM) and scanning electron microscopy (SEM). At a laser fluence of 0.9Jcm−2, interaction between Ni and Ti layers was initiated, and NiTi alloy formed in 5- and 10-bilayered samples. Progressed alloying was achieved at a laser fluence of 1.2Jcm−2. The alloy was formed mostly within the heat affected zone (HAZ) of the sample. Surface segregation of titanium was followed by formation of a 25nm thin TiO2 film on the surface of the multilayered structures. In addition, parallel periodic surface structures on the surfaces of the 5- and 10-bilayered samples were clearly recorded. Their period in the case of the 5-bilayered system (0.77μm) agrees very well with the predictions of the common theory, whereas, in the case of the 10-bilayered system, two periods of such structures are observed (1.43μm and 0.4μm), and none of them coincides with the prediction.