An improved pyroelectric material comprises a polycrystalline material doped with at least one donor element such that the polycrystalline material has a grain size less than 10 .mu.m (or 5 .mu.m) and a Figure of Merit greater than 90 nC/(cm.sup.2.K). In the preferred embodiments the polycrystalline material is barium strontium titanate or calcium-substituted barium strontium titanate. The donor element may be Nb, Ta, Bi, Sb, Y, La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er or a combination thereof. The material may additionally be doped with an acceptor such as Co, Cu, Fe, Mn, Ru, Al, Ga, Mg, Sc, K, Na, U, In, Mg, Ni, Yb or a combination thereof to control the resistivity. Other structures and methods are also disclosed.