Bulk rock geochemistry and SWIR reflectance spectroscopy are widely used by companies for rapid and cost-effective exploration of volcanic-hosted massive sulfide (VHMS) deposits. However, few studies have integrated bulk-rock geochemistry with hyperspectral reflectance spectroscopy in greenstone belts that have undergone high-grade metamorphism. Here we present an extensive dataset combining bulk-rock geochemistry with chlorite and white mica SWIR spectral reflectance from the amphibolite-grade King VHMS deposit of the Yilgarn Craton, Western Australia. At King, the footwall stratigraphy is dominated by tholeiitic mafic rocks overlain by a sequence of calc-alkaline intermediate-felsic metavolcanic rocks. The hanging-wall stratigraphy is characterized by a thin metaexhalite layer, overlain by thick succession of interbedded metasedimentary and metavolcanic rocks. Chlorite spectral signatures are more Fe-rich in mafic lithologies and Mg-rich in felsic rocks, particularly where intense Mg-metasomatism occurred before metamorphism. In all units, Fe/Mg ratios of chlorite are strongly tied to bulk rock Fe/Mg ratios. White mica in the footwall is primarily muscovitic, with minor amounts of phengite in deep Fe-rich mafic rocks. By contrast, the hanging-wall sequence is dominated by phengitic signatures in both the Fe-rich metaexhalite, and weakly Ca-Mg altered volcanic rocks. This study concludes that chlorite SWIR reflectance is largely influenced by the bulk Fe/Mg composition of the host rock, whereas white mica reflectance correlates with the type and intensity of hydrothermal alteration prior to metamorphism. These findings underscore the potential of using chlorite and white mica spectral signatures to understand hydrothermal alteration patterns and detect new orebodies in metamorphosed VHMS systems.