Ions doping-driven structural phase transition accompanied by magnetism switching and band-gap narrowing effects has been observed in PbTi 1Àx Ni x O 3Àd (xPTNO, x ¼ 0.00, 0.06, and 0.33) thin films. With the increase of x, the xPTNO thin films exhibit not only a phase transition from the pseudotetragonal structure to a centrosymmetric cubic structure but also a drastic decrease of grain size. Moreover, the as-grown Ni-doped PbTiO 3 (PTO) thin films show obvious room-temperature ferromagnetism and an increased saturation magnetization with increasing the Ni content, in contrast to undoped PTO, which shows diamagnetism. A bound magnetic polaron model was proposed to understand the observed ferromagnetic behavior of PTO-derived perovskite thin films. Furthermore, the 0.33PTNO thin film presents a narrowed band-gap, much smaller than that of PTO, which is attributed to new states of both the highest occupied molecular orbital and the lowest unoccupied molecular orbital in an electronic structure with the presence of Ni. These findings may open up a route to explore promising perovskite oxides as candidate materials for use in multiferroics and solar-energy devices. V C 2015 AIP Publishing LLC. [http://dx.