The pyroelectric coefficients of 0.72Pb(Mg1∕3Nb2∕3)O3-0.28PbTiO3 (PMN-28PT), 0.67Pb(Mg1∕3Nb2∕3)O3-0.33PbTiO3 (PMN-33PT), and 0.92Pb(Zn1∕3Nb2∕3)O3-0.08PbTiO3 (PZN-8PT) single crystals, oriented and poled along three different crystallographic directions, [001]C, [011]C, and [111]C, have been measured using a dynamic method. The suffix C indicates reference to the prototypic cubic coordinate system. Large coefficients of up to 1070μCm−2K−1 have been observed for the [111]C oriented, rhombohedral PMN-28PT and PMN-33PT samples, where the measurement direction corresponds to the polar axis of the crystal. For each composition and orientation two different poling procedures are compared, a commonly used field cooling method and a low temperature poling protocol. It was found that in otherwise pseudoorthorhombic samples of PZN-8PT, a room temperature rhombohedral phase could be stabilized by application of a field along the [111]C direction while heating from −70°C.