The explosive advances in modern communication have provoked huge requirements for microwave devices with superior performance. To satisfy the criteria for device fabrication, microwave dielectric ceramics should own a proper dielectric constant (ε r ), a high-quality factor (Qf), and a nearzero temperature coefficient of resonant frequency (τ f ). [1][2][3] Recently, low-temperature co-fired ceramic (LTCC) technology has gained considerable attention for it can effectively lessen the volume of components, allowing for realizing miniaturization, integration, and modularization of devices. In LTCC, ceramics need to be co-fired with metal electrodes (e.g., Ag), which requires a low sintering temperature (ST) (<961°C, the melting point of Ag) and chemical compatibility with electrodes. [4][5][6] There are numerous ceramic systems developed with desirable properties, such as MgO-