This work prepared a novel Sr2CaMoO6 (SCM) ceramic through the conventional solid-state process. The crystal structure, chemical bond characteristics, and microwave dielectric properties of SCM ceramic were investigated for the first time. The X-ray diffraction patterns and Rietveld refinement indicate that SCM ceramic formed an orthorhombic phase with the space group Pmm2 (25) at temperatures above 1300 °C. The lattice vibrational modes of SCM ceramic were obtained through the Fourier transformed infrared spectrum (FTIR). The measured dielectric constant and dielectric loss of SCM ceramic is close to the theoretical values obtained by FTIR. According to the P–V–L theory, the chemical bond characteristics of SCM ceramic were calculated. The high ionicity and lattice energy of the Mo–O bond positively affect the properties of SCM ceramic. The outstanding microwave dielectric properties of εr = 19.37, Q·f = 32,970 GHz (at 5.96 GHz), and τf = −32.56 ppm/°C were obtained in SCM ceramic sintered at 1450 °C. This work reveals the crystal structure of SCM ceramic, establishes the relationship between the properties and chemical bonds of the ceramic, and lays a foundation for studying the dielectric properties of related ceramic systems.