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The electric and dielectric properties of Na0.5Bi4.50+xTi4Oy (x = −0.02, 0, 0.02) prepared by conventional mixed oxide route have been investigated by impedance spectroscopy (IS) over a wide temperature range. Single‐phase bismuth layer‐structured perovskite patterns were observed through X‐ray diffraction of the three samples Na0.5Bi4.5Ti4O15, Na0.5Bi4.48Ti4Oy, and Na0.5Bi4.52Ti4Oy. The results show that the relative permittivity (εr) increases with the increase in temperature and reaches its maximum at about 675℃. With the continuous increase in temperature, the permittivity decreases gradually. Both relative permittivity and dielectric loss show great stability at the low‐temperature zone. The ceramic of x = 0.02 with Ea of 1.09 eV has the maximum oxygen ionic transport number between 600 and 800℃ for all samples. And at this time, it has the maximum electrical conductivity. All the results indicated that Na0.5Bi4.50+xTi4Oy (x = −0.02, 0, 0.02) ceramics were promising base materials for high‐temperature capacitor because of their high dielectric properties. [ABSTRACT FROM AUTHOR]