phenomenon. [12][13][14][15] However, no experimental evidence was provided to exclude the light-induced photothermal effect and incontrovertibly demonstrate the existence of light-induced spin transitions in these metal-oxide systems. More importantly, it is noted that the photogenerated electrons in transition metal oxides are free to roam within the solid, [16,17] preventing them from directly altering the metal centers' spin configuration via localization on a single atomic site. This fundamental difference between material systems casts doubt over the validity of adopting the steady-state spin transition theory to describe photomagnetism in nanoparticlebased magnets.In this contribution, we examined the magnetic response of superparamagnetic Fe 3 O 4 nanoparticles following photoexcitation and found that the exciton-spin exchange-coupling interaction is the primary mechanism by which this archetypal transition metal oxide exhibits photomagnetism. Studying the photomagnetic response at temperatures below the blocking temperature under various external fields revealed that the exciton-spin exchange-coupling interaction reduces the magnetic energy barrier governing spin-flip transitions within iron oxide nanoparticles, allowing an optically driven magnetic phase transition from ferrimagnetic to superparamagnetic when held in their "blocked" state and a corresponding decrease in their saturation magnetization. Further investigation showed a significant decrease in photomagnetism as the Fe 3 O 4 nanoparticle size was increased, pinpointing the critical role of restricting the nanoparticle's magnetic anisotropy in enabling photomagnetism. Significantly, we have excluded light-induced photothermal heating as the source of photomagnetism in Fe 3 O 4 nanoparticles by comparing experimentally measured magnetization changes with those predicted from theoretical simulations based on a photothermal mechanism. Taken together, our findings provide fundamental insights into the origin of photomagnetism in transition metal oxides and establish a deeper understanding of the underlying mechanism that regulates the light-induced spin dynamics in iron oxide nanoparticles.High-resolution transmission electron microscopy (HRTEM) reveals that spherical nanoparticles were produced with an average size of 7.0 ± 1.0 nm (Figure 1a, also see Figure S1a,b in the Supporting Information). X-ray photoelectron spectroscopy Using light irradiation to manipulate magnetization over a prolonged period of time offers a wealth of opportunities for spin-based electronics and photonics. To date, persistent photomagnetism has been frequently reported in spin systems composed of molecular magnets; yet this phenomenon is rarely observed in nanoparticle-based systems comprised of transition metal oxides. Here, detailed studies of persistent photomagnetism in superparamagnetic iron oxide (Fe 3 O 4 ) nanoparticles at temperatures below their blocking temperature are presented and it is demonstrated that the magnetization change does not occur through stea...