In ancient basement regions such as the Lewisian Complex, NW Scotland, the ages of brittle deformation events are commonly poorly constrained owing to a lack of datable fills. An array of NW–SE sinistral and antithetic east–west dextral faults related to a regionally recognized episode of brittle shearing cut Neoarchean gneisses and c. 2.25 Ga quartz–pyrite veins close to the trace of an unexposed, regional-scale NW–SE fault. Copper–iron mineralization occurs at an intersection between an antithetic dextral fault and an older c. 2.25 Ga quartz vein. Optical microscopy, SEM and XRD analyses reveal an array of intergrown, co-genetic copper–iron sulfides, hematite and barite. Complex millimetre-thick zoned alteration rims rich in epidote occur at contacts between the sulfides and gneisses. Rhenium–osmium copper–iron sulfide geochronology yields an age of c. 1.55 Ga for the hydrothermal mineralization event associated with faulting. Fault movements demonstrably overlap with mineralization based on the asymmetric fibrous growth forms of these minerals within local dextral shears, which acted as local channelways for mineralizing fluids during and after faulting. We tentatively propose that this regionally recognized strike-slip faulting, previously termed the ‘Late Laxfordian’, should be referred to as the ‘Assyntian’ to distinguish it from kinematically distinct Laxfordian events.