The present laboratory study using high-resolution reflectance spectroscopy (0.25--2.7 μm) focuses on two primary phyllosilicate groups, serpentines and chlorites. The results show that it is possible to spectrally distinguish between isochemical end-members of the Mg-rich serpentine group (chrysotile, antigorite, and lizardite) and to recognize spectral variations in chlorites as a function of Fe/Mg ratio (~8--38 wt % Fe). The position and relative strength of the 1.4-μm absorption feature in the trioctahedral chlorites appear to be correlated to the total iron content and/or the Mg/Si ratio and the loss on ignition values of the sample. Spectral differences in the 2.3-μm wavelength region can be attributed to differences in lattice environments and are characteristic for specific trioctahedral chlorites. The 1.4-μm feature in the isochemical Mg-rich serpentines (total iron content ~1.5--7.0 wt %) show marked spectral differences, apparently due to structural differences.