Abstract Layered structures comprising high-coupling lithium niobate (LiNbO3, LN) piezoelectric thin plates bonded to high-velocity SiC substrates have attracted much attention of high-performance surface acoustic wave (SAW) devices. However, such these layered structures exhibit severe Rayleigh mode spurious responses that degrade the performances of SAW devices. This paper explores the generation mechanism of spurious modes on LN/SiC layered structure, and proposes an optimized layered structure with suppressed Rayleigh spurious modes. The investigation involves deriving the Euler angle range of LN by analysing the slowness surface of both LN and SiC. In addition, it is worth noting that slowness surface overlaps at some Euler angle ranges, which will cause coupling between different modes, thus generating spurious mode. Simulation result shows the frequency characteristics of SAW resonator at resonant and anti-resonant frequencies of 4.3 GHz and 4.88 GHz of SH mode, achieving a K 2 of up to 26.5% and a quality factor Q of 828. It is proved that the optimization structure offering larger K 2, higher velocity and improved Q values and Rayleigh spurious mode suppression, which is favourable for wideband and high frequency SAW devices applications.