Exposures of Archean rocks older than 3.5 Ga are rare, such that investigations of the earliest felsic continental crust are limited to specific regions (e.g., the Acasta Gneiss Complex in the Slave Craton in Canada and the Isua Greenstone Belt in Greenland). In this work, we present new in situ apatite, titanite, and zircon U–Pb data in conjunction with textural observations for comparatively underexplored rocks from the Sylvania Inlier, Pilbara Craton, Western Australia, that provide a window into the timing and processes of early Paleoarchean crust production. The studied rocks are characterized by a mix of felsic domains with quartz–plagioclase assemblages and mafic domains with hornblende–epidote–titanite–ilmenite–plagioclase assemblages. The felsic domains are interpreted to represent leucosomes and have a weighted mean 207Pb/206Pb zircon age of ~3575 Ma, which necessitates partial melting of an even older mafic protolith. Titanite rims around ilmenite cores yield a weighted mean 207Pb/206Pb titanite age of ~3540 Ma, suggesting that titanite growth was near coeval with partial melting. Apatite U–Pb data indicate that this rock cooled below the Pb blocking temperature (~450 °C) at ~2800 Ma. These new results imply that the Sylvania Inlier is a suitable natural laboratory to examine some of the oldest differentiation processes documented on Earth.