High-density well-aligned ZnO nanorods were successfully synthesized on ZnO-buffer-layer coated indium phosphide (InP) (100) substrates by a pulsed laser deposition (PLD) method. Scanning electron microscopy images show that the ZnO buffer layer formed uniform drip-like structure and ZnO nanorods were well-oriented perpendicular to the substrate surface. The sharp diffraction peak observed at 34.46° in X-ray diffraction scanning pattern suggests that the ZnO nanorods exhibit a (002)-preferred orientation. The PL spectra of ZnO samples shows a strong near band edge emission centered at about 380 nm and a weak deep level emission centered at around 495 nm, and it demonstrates that the ZnO nanorods produced in this work have high optical quality, which sheds light on further applications for nanodevices.ZnO, nanorods, buffer-layer, self-catalyst, pulsed laser deposition In recent years, semiconductor nanostructures have attracted much attention due to their potential applications in a wide range of advanced devices. Among these nanostructures, ZnO nanostructures arrays have been considered to be the most prospective one due to its direct wide band gap of 3.37 eV and a large exciton binding energy of 60 meV [1] , which has been recognized as a promising candidate for applications in functional oxide-based. Additionally, it may be used for electromechanical coupled sensors, transducers and biomedical applications [2][3][4] , because of its piezoelectric and biocompatible properties, respectively. Furthermore, various techniques are employed to fabricate ZnO nanostructures, such as chemical vapor deposition (CVD) [5] , metal-organic chemical vapor deposition (MOCVD) [6] , thermal evaporation [7] , molecule beam epitaxy (MBE) [8] , and pulsed laser deposition (PLD) [9] . Therefore, ZnO nanostructures have attracted so much attention, and a large number of publications have been presented recently for reporting ZnO nanostructures with diverse morphologies grown by different approaches. Wang et al. [10] and Gao et al. [11] demonstrated the synthesis of ZnO nanostructures by a solid-vapor phase thermal sublimation technique. This approach is the most widely used technique for synthesizing aligned ZnO nanostructures, in which the assistance of metal catalysts are frequently chosen, such as Au, Co, and Cu, commonly introducing impurities in the products. Consequently, it is necessary to develop catalyst-free growth techniques of ZnO nanostructures. Vayssieres [12] grew arrayed ZnO nanorods and nanowires by a catalyst-free aqueous solutions method. Chen et al. [13] also synthesized flower-like ZnO nanorods by a catalyst-free sonochemical method. However, there is no report about self-catalyst preparing ZnO nanostructures by a PLD technique.As we known, only sparse ZnO nanostructures were prepared on InP substrates by a PLD method. The main