Chlorite is one of the most common Fe-bearing minerals and is susceptible to weathering in loess and soils. The conventional method for analyzing chlorite, based on XRD with the Rietveld technique, is quantitative, but very time consuming and expensive. In this paper we develop a new methodology based on diffuse reflectance spectroscopy (DRS) and selective chemical extractions to identify chlorite qualitatively in the Chinese loess sequence and present evidence suggesting that DRS may be used to quantify chlorite content. The spectral signature of chlorite in loess is obscured by Fe oxides, but becomes obvious when they are removed. Changes in the ferrous absorption band near 1140 nm vary consistently with changing chlorite content. Using this spectral feature, DRS can distinguish chlorite contents as small as 1 wt.% in loess sediments. Future possibilities for this method in other soil and sediment types need to be explored.