In this study, a series of rare‐earth titanates with the general formula Re2TiO5 (Re = Er, Tm, Yb, and Lu) were synthesized and their microwave dielectric properties were reported. The impact of differences in rare‐earth cation radii on the structure and dielectric properties was systematically analyzed. The findings indicated that ceramics of Re2TiO5 (Re = Er, Tm, Yb, and Lu) were crystallized into a cubic structure with space group Fd‐3m, as confirmed by Rietveld refinement and selected‐area electron diffraction patterns. The rare‐earth elements were analyzed for their impact on microwave dielectric properties, considering factors such as ionic polarizability, packing fraction, and bond valence theory. The resulting materials exhibited excellent microwave dielectric properties with a low permittivity (6.95–7.21), high‐quality factors (19 451–20 115 GHz), and low positive temperature coefficient of resonance frequency (19.34–20.90 ppm/°C). The origin of low permittivity was elucidated through the analysis of bond length, X‐ray photoelectron spectroscopy, and impedance spectroscopy. This series of titanates exhibited unusually low permittivity characteristics in the microwave frequency range, which could meet the low signal transmission delay requirements in wireless communication.