In this paper, a novel low-temperature sintering substrate for low temperature co-fired ceramic applications based on indialite/cordierite glass ceramics with Bi2O3 as a sintering aid showing low permittivity (εr) and ultralow dielectric loss (tan δ) is described. The fine powder of indialite was prepared by the crystallization of cordierite glass at 1000 °C/1 h. The optimized sintering temperature was 900 °C with 10 wt % Bi2O3 addition. The relative density achieved was 97%, and εr and tan δ were 6.10 and 0.0001 at 1 MHz, respectively. The composition also showed a moderately low temperature coefficient of relative permittivity of 118 ppm/°C at 1 MHz. The obtained linear coefficient of thermal expansion was 3.5 ppm/°C in the measured temperature range of 100 to 600 °C. The decreasing trend in dielectric loss, the low relative permittivity at 1 MHz, and the low thermal expansion of the newly developed composition make it an ideal choice for radio frequency applications.