In this study, aligned porous lead zirconate titanate (PZT) ceramics with high pyroelectric figures-of-merit were successfully manufactured by freeze casting using water-based suspensions. The introduction of aligned pores was demonstrated to have a strong influence on the resultant porous ceramics, in terms of mechanical, dielectric, and pyroelectric properties. As the level of porosity was increased, the relative permittivity decreased, whereas the Curie temperature and dielectric loss increased. The aligned porous structure exhibited improvement in the compressive strength ranging from 19 to 35 MPa, leading to easier handling, better processability and wider applications for such type of porous material. Both types of pyroelectric harvesting figures-of-merit (F E and F 0 E ) of the PZT ceramics with a porosity level of 25-45 vol% increased in all porous ceramics, for example, from 11.41 to 12.43 pJ/m 3 / K 2 and 1.94 to 6.57 pm 3 /J, respectively, at 25°C, which were shown to be higher than the dense PZT counterpart.