Mixed-layered phyllosilicates with composition intermediate between mica and chlorite were identified in very low-grade metaclastites from the Maláguide Complex (Betic Cordilleras, Spain), and studied by X-ray diffraction, and transmission and analytical electron microscopy. They occur both as small grains in the rock matrix, and associated with muscovitechlorite stacks. Transmission electron microscope observations revealed a transition from chlorite to ordered 1:1 interstratifications through complex 1:2 and 1:3 interstratifications. Analytical electron microscopy data indicate a composition slightly different from the sum of discrete trioctahedral chlorite and dioctahedral mica. The types of layer transitions suggest that mixed-layer formation included two main processes: (1) the replacement of a brucite sheet by a cation sheet in the chlorite structure; and (2) the precipitation of mica-like layers between the chlorite layers. The strongest diffraction lines in oriented X-ray patterns are: 12.60 Å (002), 7.98 Å (003), 4.82 Å (005) and 3.48 Å (007).