To obtain both high power durability and fine-dimensional control in high-frequency surface acoustic wave devices, a highly oriented (111) texture was developed in electronic beam evaporated Al films on Zr underlayer. In this paper, the effects of Zr underlayer on the microstructure and resistivity of Al/Zr/LiNbO3 films were investigated. The films show an extremely smooth surface. The optimum annealing temperature is 200 °C to obtain low resistivity. For Al films with Zr underlayer, reactive ion etching with gases containing BCl3 can be more easily performed than that for Al films with Cu underlayer.