a- and b-axis-oriented (Bi3.25Nd0.75−
x
Eu
x
)Ti3O12 (BNEuT, x = 0–0.75) films of 3.0 µm thickness were fabricated on conductive Nb:TiO2(101) substrates containing 0.79 mass % Nb by high-temperature sputtering at 650 °C, and their structural and piezoelectric characteristics were investigated. The room-temperature remanent polarization (2P
r) and effective piezoelectric coefficient (d
33) values for the BNEuT films exhibited maxima of 87 µC/cm2 and 15 pm/V, respectively, at x = 0.10, which were approximately 1.3 times larger than those (2P
r = 65 µC/cm2 and d
33 = 12 pm/V) of the nondoped (Bi3.25Nd0.75)Ti3O12 (BNT) nanoplate. The BNEuT film with x = 0.10 had a high a-axis orientation judging from the X-ray diffraction measurement and the observation of the phase image by piezoresponse force microscopy. It is shown that adequate Eu3+ doping of BNT nanoplates produces a larger displacement magnitude of the octahedra than that in the nondoped BNT nanoplate, resulting in an improvement of piezoelectric properties in addition to the ferroelectricity.