Nonstoichiometry lead-free 0.94Na x Bi y TiO 3 -0.06Ba z TiO 3 (N x B y T-0.06B z T) (from x = y = 0.5, z = 1.00 to x = 0.5, y = 0.534, z = 1.02) ceramic compositions were prepared by a conventional solid-state route. XRD shows that the compositions are at a morphotropic phase boundary where rhombohedral and tetragonal phases coexist. The depolarization temperature (T d ) can be lowered by modifying x, y and z. The pyroelectric coefficient (p) of nonstoichiometry N x B y T-0.06B z T compositions is greatly increased, compared with stoichiometry NBT-0.06BT composition, from 3.15 9 10 -4 C m -2°C-1 at room temperature (RT) and 23.9 9 10 -4 C m -10 m v -1 , 0.39 9 10 -10 m 2 C -1 and 138.7 9 10 -6 Pa -1/2 , respectively, at T d . The same composition also presents F C values which are *2.58 and *2.86 (910 -9 C cm -2°C-1 ) at RT at 100 and 1000 (Hz). N 0.5 B 0.534 T-0.06BT and N 0.5 B 0.534 T-0.06B 1.02 T compositions show a large p values at a wide temperature range. The enhanced pyroelectric properties make nonstoichiometry N 0.52 B 0.52 T-0.06BT composition a promising candidate for pyroelectric and other applications at wide temperatures range.