The pyroelectric properties of Mn-doped Aurivillius ceramics with different pseudo-perovskite layers were investigated. The pyroelectric coefficients for 0.2 wt% Mn-doped two-layer CaBi 2 Nb 2 O 9 (CBN-Mn), three-layer Bi 4 Ti 2.85 Nb 0.15 O 12 (BTN-Mn), and four-layer CaBi 4 Ti 3.95 Nb 0.05 O 15 (CBTN-Mn) ferroelectric ceramics were found to be on the order of 26.0, 54.4, 84.4 μC/m 2 K at room temperature, respectively. These values were closely associated with the number of octahedral layers in the pseudo-perovskite blocks. The high pyroelectric coefficient, together with low dielectric permittivity and loss (tan δ < 0.003), results in to high figures of merit for the current responsivity, voltage responsivity, and detectivity. The excellent pyroelectric properties and high Curie temperatures (T C > 660°C) make the Aurivillius ceramics potential candidates for pyroelectric devices over a broad temperature range.