La and Ta co-doped Lead-free 0.94NBT-0.06BT ceramics were synthesized by a conventional solid-state route. The compositions remain at a morphotropic phase boundary. The depolarization temperature (Td) decreased with increasing doping contents. The room temperature (RT) pyroelectric coefficient (p) was highly enhanced compared with undoped material (3.15 x10-4 C.m-2 .°C-1) and reached 12.9 x10-4 C.m-2 .°C-1 , whereas, at Td, 58.6 x10-4 C.m-2 .°C-1 could be obtained rather than 23.9 x10-4 C.m-2 .°C-1 for undoped materials. The pyroelectric figure of merits, Fi and Fv, also showed a huge improvement from 1.12 x10-10 m.v-1 and 0.021 m 2 .C-1 of undoped material to 4.61 x10-10 m.v-1 and 0.078 m 2 .C-1 of doped materials at RT, and to 20.94 x 10-10 m.v-1 and 0.28 x10-10 m 2 .C-1 at Td. RT FC values are2 .40, 2.46, and 2.57 (x10-9 C.cm-2 .°C-1) at frequency 33, 100 and 1000 (Hz) respectively, at La = Ta = 0.2 %. The pyroelectric coefficient achieved at RT in this study is almost one order of magnitude higher than PZT materials, furthermore, the figure of merits of the new compositions are comparable with or even better in those of PZT materials and other leadfree ceramics. The improvement in the pyroelectric properties makes La and Ta co-doped NBT-0.06BT ceramics possible materials to replace lead-containing PZT ceramics for infrared detector materials at a wide temperature range.