Highly Bi-substituted neodymium iron gallium garnet thin films with a Bi content of 2.5, Nd0.5Bi2.5Fe5−
y
Ga
y
O12 (NBIGG) with y = 0–1, on gadolinium gallium garnet (111) and (100) substrates have been prepared by metal–organic decomposition. Magnetic properties and magnetic anisotropy energies were measured using an alternating field gradient magnetometer and by magnetic torque measurement, respectively. Faraday rotation spectra and hysteresis loops were measured using a Faraday rotation spectrometer. The magnetization of NBIGG thin films exhibiting a large Faraday rotation of 10–15°/µm decreased with increasing Ga content, resulting in increased effective magnetic anisotropy energy K
eff. The dependence of the magnetic anisotropies on the Ga content is discussed in terms of the reverse magnetostrictive effect caused by thermal stress as well as the magnetocrystalline and shape anisotropies.