Pillow basalt and chert form integral lithologies comprising many Archean greenstone belt packages. To investigate details of these lithologies in the >3.7 Ga Isua Greenstone Belt, SW Greenland, we measured silicon isotope compositions of quartz crystals, by secondary ion mass spectrometry, from a quartz-cemented, quartz-amygdaloidal basaltic pillow breccia, recrystallized chert and chert clasts thought to represent silica precipitation under hydrothermal conditions. The recrystallized chert, chert clasts and quartz cement have overlapping δ30Si values, while the δ30Si values of the quartz amygdules span nearly the entire range of previously published values for quartz precipitates of any age, despite amphibolite facies metamorphism. We suggest that the heterogeneity is derived from kinetic isotope fractionation during quartz precipitation under disequilibrium conditions in a hydrothermal setting, consistent with the pillow breccia origin. On the basis of the present data, we conclude that the geological context of each sample must be carefully evaluated when interpreting δ30Si values of quartz.