Electrophoresis and streaming potential data are reported for crushed and sheet muscovite mica respectively. For streaming potential measurements a newly designed radial flow apparatus was used. Measurements on crushed mica show that both aluminium and silicon leach out of the mica. Leached aluminium and silicon may readsorb to confer increased positive and negative charge respectively on the mica. Electrophoresis data indicate that leaching of aluminium occurs more rapidly than of silicon. Aging experiments on sheet mica show leaching effects to be much slower than on crushed mica. Streaming potential measurements on freshly cleaved mica sheets showed that (i) the zeta- potential depended strongly on electrolyte (KCl) concentration; (ii) the zeta-potential was relatively independent of pH and (iii) monovalent cations were adsorbed in the sequence H+ > Cs+ > K+ > Na+ > Li+, whilst Ca2+ adsorbed more strongly than K+. It is proposed that the structure of the electrical double layer at the mica/electrolyte interface results from the distribution of all ions between the diffuse layer, the Stern plane (hydrated) and more critically the lattice holes of the silica-alumina basal plane.