Mixed-layer minerals with optical properties similar to metamorphic vermiculite were identified in rocks belonging to a Palaeozoic and a Triassic formation separated by an angular unconformity and exposed in the Coastal Range of central Chile. Both formations are affected by low-grade metamorphism. The mixed-layer minerals were studied by optical microscopy, X-ray diffraction (XRD), electron microprobe (EMPA), and transmission/analytical electron microscopy (TEM/AEM). Two types of phyllosilicates were identified: chlorite-vermiculite and mica-chlorite, which are present in the Palaeozoic and Triassic rocks respectively. Chlorite-vermiculite mixed layers form packets with well-defined boundaries and mainly show 1:1 ordered sequences. On the contrary, mica-chlorite mixed layers show, in most cases, random sequences evolving laterally toward chlorite. The AEM data indicate compositions close to that of chlorite in the ternary Si-Al-(Fe+Mg+Mn) diagrams for both types of mixed-layer phyllosilicates. Relative to the coexisting chlorite, they have lower (Fe+Mg) contents, and a higher Si/Al ratio. They are interpreted as products of the transformation of chlorite, developed during prograde metamorphism, and probably represent intermediate, metastable phases, in the chlorite to biotite transformation.