AbstractIn this work, we fabricated the (1‐x)BiFeO3‐xBaTiO3+y‰ mol CuO ceramics by the modified thermal quenching technique. The pure perovskite phase was formed and a morphotropic phase boundary (MPB) was observed in the ceramics with x = 0.30‐0.33. The addition of CuO can significantly enhance the density of the BiFeO3‐BaTiO3 material. Importantly, an enhanced piezoelectric constant (d33=165 pC/N), a large electric‐field‐induced strain (∆S = 0.54%: peak to peak strain) and a large piezoelectric actuator constant (d33*=449 pm/V) together with a high Curie temperature (TC) of 503°C were observed in the ceramics with x = 0.30 and y = 5. As a result, the enhanced piezoelectricity and large electric‐field‐induced strain could significantly stimulate further researches in BFO‐based ceramics.