Abstract--Transmission electron microscopy has been used to characterize coexisting pyrophyllite and muscovite in low-grade metamorphosed pelites from Witwatersrand and northeastern Pennsylvania. The Witwatersrand sample consisted largely of porphyroblasts of interlayered muscovite and pyrophyllite in a fine-grained matrix of the same phases. In both textures, muscovite and pyrophyllite occurred as interlayered packets (with apparently coherent interfaces) from about 300 A to a few micrometers in thickness, with no mixed layering. Their compositions were determined with a scanning transmission electron microscope to be (Do.H KL72NaoA 7)(A13.9 ~ Feo.03Mgo.osTio.01)(Si6.1 ~ All.s9)O20(OH)4 and (D t.90Nao.06Ko.oa)(A13.gaFeo.ot Mgo.os)(SiT.94Alo.06)O20(OH)4, respectively.The pyrophyUite and muscovite in the Pennsylvania shale likewise occurred only as coexisting coherent to sub-parallel packets as thin as 200 ~, with compositions of ([-ql.s9Nao.04Cao.02Ko.05)(A13.93Feo.04Mgo.02Tio.oj)(Si7.92Alo.os)O20(OH)4 and (Nao.o,fao.02K2.03XA13.saFeo.24Mgo.~6Tio.06)(Si6.09Al Lg~)O20(OH),. The textures of both samples were consistent with an equilibrium relationship between pyrophyllite and muscovite. The Pennsylvania sample also contained N H 4 -r i c h illite, kaolinite, and an illite-like phase having intermediate Na/K, which collectively imply non-equilibrated low-grade conditions.The compositions of these coexisting pyrophyllite and muscovite define a solvus with steep limbs and extremely limited solid solution. Illite is a white mica, intermediate in composition between pyrophyllite and muscovite, formed at much lower temperatures than muscovite. These relations show that illite is metastable relative to pyrophyllite + muscovite in all of its diagenetic and low-grade metamorphic occurrences. This further implies that illite precursor phases, such as smectite, are also metastable. The prograde reactions involving smectite, illite, and muscovite are therefore inferred to represent Ostwaldstep-rule-like advances through a series of metastable phases toward the equilibrium states attained in the greenschist facies. "Illite crystallinity" can therefore be a measure of reaction progress, for which temperature is only one of several determining factors.