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The magneto-optical signatures of colloidal noble metal nanostructures, spanning both discrete nanoclusters (<2 nm) and plasmonic nanoparticles (>2 nm), exhibit rich structure-property correlations, impacting applications including photonic integrated circuits, light modulation, applied spectroscopy, and more. For nanoclusters, electron doping and single-atom substitution modify both the intensity of the magneto-optical response and the degree of transient spin polarization. Nanoparticle size and morphology also modulate the magnitude and polarity of plasmon-mediated magneto-optical signals. This intimate interplay between nanostructure and magneto-optical properties becomes especially apparent in magnetic circular dichroism (MCD) and magnetic circular photoluminescence (MCPL) spectroscopic data. Whereas MCD spectroscopy informs on a metal nanostructure's steady-state extinction properties, its MCPL counterpart is sensitive to electronic spin and orbital angular momenta of transiently excited states. This review describes the size- and structure-dependent magneto-optical properties of nanoscale metals, emphasizing the increasingly important role of MCPL in understanding transient spin properties and dynamics.