This research was conducted to study the effect of ZnO nano-particulate modification on properties of Pb(Zr0.52Ti0.48)O3 (PZT)-(Bi3.25La0.75)Ti3O12 (BLT) ceramics prepared by a mixed-oxide solid-state sintering method. ZnO nano-particulate was added into PZT-BLT ceramics to obtain PZT-BLT/xZnO (x = 0, 0.1, 0.5 and 1.0 wt%). The PZT-BLT/xZnO ceramics were investigated in terms of phase, microstructure, physical, electrical, and mechanical properties. Tetragonality of PZT-BLT crystal structure tended to increase with increasing ZnO content. ZnO addition obviously increased the density of PZT-BLT ceramics while the grain size slightly decreased. Intergranular fracture mode was observed for pure PZT-BLT ceramic while the samples contained ZnO nano-particles showed a mixed-mode inter-/trans-granular fracture. Addition of ZnO also affected hardness and fracture toughness values. Addition of ZnO nano-particulate into PZT-BLT ceramics was found to improve room temperature dielectric constant but did not have a significant effect on ferroelectric properties. These observed results were expected to be caused by the behaviors similar to a donor-doped system. © 2011 Elsevier Ltd and Techna Group S.r.l.