his paper is concerned with the FR spectra analysis on the Bi, Tb and Yb partially substituted iron garnet crystals of Tb3-x-yYbyBixFe5O12. A specific FR (-1617o/cm at 1.55μm), a low FWC (0.009%/nm at 25oC) of Tb0.91Yb1.38Bi0.71Fe5O12 crystals grown from Bi2O3 self-fluxed melts can be used as broadband optical communication components. In order to interpret their FR spectra, a theory based on molecular-orbital levels of Fe3+ in tetrahedral and octahedral sites is used. It is shown that in the case of higher Bi3+ substitution, FR is mainly determined by the contribution of Fe3+ in the octahedral site. Furthermore, two types of rare-earth ions (Tb3+ and Yb3+) moderate the contribution to FR from Fe3+ in octahedral and decahedral sites and eventually have caused that Bi-substituted mixed rare-earth iron garnet has a near-zero Faraday rotation wavelength coefficient (FWC).