Pyroelectric properties of phosphoric acid (H3PO4)-doped triglycine sulfate (TGSP) single crystals grown from solutions containing 0.1–0.5 mol of H3PO4 have been studied. Incorporation of H3PO4 into the crystal lattice is found to induce an internal bias field (Eb) and is observed through the presence of a sustained polarization and pyroelectricity beyond the transition temperature. The internal bias field has been estimated theoretically by fitting the experimentally measured data on temperature dependence of the pyroelectric coefficient (λ), dielectric constant (ε′) and polarization (P). A high Eb value in the range 9 × 103–15.5 × 104 V m−1 is obtained for crystals grown with 0.1–0.5 mol of H3PO4 in the solution, and a specific concentration of 0.2–0.25 mol of H3PO4 in the solution during crystal growth is found to be optimum for a high figure of merit for detectivity, Fd = 428 µC m−2 K−1.