The performance of ZnO/64°-YX LiNbO3 and ZnO/36°-YX LiTaO3 layered SAW structures was compared in terms of mass sensitivity and acoustic wave velocity. It was found that the ZnO/64° LiNbO3 structure has a few distinct advantages over ZnO/36° LiTaO3. For ZnO/64° LiNbO3, the mass sensitivity is similar to 2.5 times larger. Additionally, the optimum thickness of the ZnO guiding layer is approximately half that of the ZnO/36° LiTaO3 structure, which reduces the cost of fabrication.