The effects of different concentrations of Mn2+, Mg2+, Al3+, Fe3+, La3+, and Nb5+ on the dielectric and tunable properties of Ba0.6Sr0.4TiO3 ceramics were investigated. It was found that doping in small amounts with acceptor ions such as Mg2+, Fe3+, and Al3+ could meliorate the dielectric properties clearly. Decrease of dielectric loss was attributed to the formation of compensating defects originating from acceptor substitution. It was concluded that the tunability was linked to both the dielectric constant and the grain size. A higher figure of merit was obtained by doping the ceramics with smaller ions of Al and Fe, compared to Ti.