Lattice dynamics and dielectric behavior in a wide frequency range of Ba0.4Sr0.6−yMnyTiO3 ceramics were investigated by using infrared (IR) spectroscopy and dielectric measurements. X‐ray diffraction results revealed that only perovskite phase was visible for all compositions. Mn occupied A‐site preferably as Mn2+ when y ≤ 0.02; whereas when y ≥ 0.05, Mn occupied B‐site and was oxidized to Mn3+. Dielectric measurements and IR analysis indicated that the hardening of the softest mode was not remarkable with increasing Mn concentration, which resulted in an unremarkable change in tunability. Compared to the samples with y ≤ 0.02, those with y ≥ 0.05 had a higher fitted damping factor, resulting from the distortion of the perovskite lattice caused by the incorporation of Mn at the Ti‐site, which led to a low intrinsic quality factor.