The electrical transport behaviors of novel materials under the external magnetic field , especially the large or tunable magnetoresistance (MR) effect, are of broad importance in both fundamental science and applications. Here three kinds of crystals with varied Te-deficiency concentrations are synthesized under different growth conditions, and they demonstrate distinct electrical and magnetotransport properties. The temperatures of the resistivity cusp or MR cusp of the as-grown (, 0.08, 0.13) crystals are tuned from 25 to 90 K. The maximum MR of these three crystals, under 2 K and 9 T , are , , and for sample SI (), SII (), and SIII (), respectively. The fitting of Hall data by the two-carrier model suggests that the extremely large MR effect of sample measured at 2 K is attributed to the cooperative action of the high mobility and the coexistence of the electron and hole carriers. Our work provides a viable route to tune superior MR properties in similar compounds through defect engineering, which may be promising to develop magnetic memory sensor devices.