Combinatorial experiments are achieved on periodically structured Ni-Ti thin film composition spreads by laser interference irradiation using a Nd:YAG laser. Continuous Ni-Ti compositional spreads covering almost the whole binary system are prepared by combining sputter mask, shutter and movement of substrate. The continuous compositional spread is subsequently micro-structured into a sample library consisting of well-defined lines of individual samples by laser interference irradiation. The composition and microstructure effects in continuous spread and sample libraries after laser structuring are explored by scanning electron microscopy (SEM) with energy dispersive spectroscopy (EDS), X-ray diffraction (XRD) and white light interferometry (WLI) microscopy. The sample library consists of individual samples with a distance of about 5 mu m and a composition resolution as high as 0.1 at.% in between. Although, there are certain difficulties so far in obtaining the optimized laser fluence for the spread, the laser interference irradiation provides an effective way to prepare thin film libraries with around 200 sample lines within 1 mm. (c) 2005 Elsevier B.V. All rights reserved.