In this work, phase-pure Mg1.8(Ni1–x
Co
x
)0.2Al4Si5O18 (0 ≤ x ≤ 1) ceramics were synthesized by a high-temperature solid-state
method. On the basis of Rietveld refinement data of X-ray powder diffraction
and Phillips–Vechten–Levine theory, the atomic ionicity,
lattice energy, and bond energy of the compound were calculated to
explore their influence on the microwave dielectric properties of
ceramics. The Mg1.8Ni0.1Co0.1Al4Si5O18 (x = 0.5) ceramic
exhibited the best microwave dielectric properties: ε
r = 4.44, Qf = 73 539 GHz@13 GHz,
and τf = −23.9 ppm/°C. (Ni1–x
Co
x
)2+ complex
ionic doping, compared with only Ni2+ or Co2+, is beneficial for improving the symmetry of [Si4Al2O18] hexagonal rings and reducing distortion. Subsequently,
8 wt % TiO2 was added to Mg1.8Ni0.1Co0.1Al4Si5O18, resulting
in a near-zero τ
f and high Qf values for the composite ceramic, with ε
r = 5.22, Qf = 58 449 GHz@13 GHz,
and τf = −2.06 ppm/°C. Finally, a 5G
millimeter-wave antenna with a central operating frequency of 25.52
GHz was designed and fabricated using the Mg1.8Ni0.1Co0.1Al4Si5O18-8 wt %
TiO2 ceramics. Operating in the 24.7–26.0 GHz range,
it demonstrated favorable radiation characteristics with a simulated
efficiency of 85.2% and a gain of 4.58 dBi. The antenna’s performance
confirms the high potential of the cordierite composite for application
in 5G communication systems.