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Abstract Realization of large effective phonon magnetic moment in monolayer MoS₂has established an important route for exploring intriguing magnetic phenomena in a nonmagnetic material. The sizable coupling between the orbital transition and the circularly polarized phonon results in the large effective phonon magnetic moment. In this work, using magneto-Raman spectroscopy, we investigate substitutional doping of magnetic atoms as a tuning knob of the electronic and phononic properties of MoS₂. We show that Fe-doping polarizes the spin of the conduction bands and introduces a localized Fe band underneath the conduction band. As a result, an additional orbital transition between the Mo 4dand Fe 3dstates emerges, producing an orbital-phonon hybridized mode at 283 cm⁻¹. Our magnetic field dependent measurements demonstrate that this new mode carries 2.8 ${\mu }_{\mathrm{B}}$effective phonon magnetic moment, which is comparable to that of the undoped MoS₂. Moreover, even though a long-range magnetic order is absent in Fe-doped MoS₂, the local magnetic moment of Fe modifies the nature of the spin fluctuation, producing monotonically increasing quasielastic scattering spectral weight as temperature decreases. Our results highlight two-dimensional dilute magnetic semiconductors synthesized by substitutional doping as a promising material platform to manipulate the phonon magnetic moment through orbital-phonon coupling.