The Neoproterozoic-Cambrian Wales Group and Ordovician-early Silurian Moira Sound unit of Prince of Wales Island, Alaska, USA, host numerous volcanic-hosted massive sulfide (VHMS) deposits and occurrences, including the Niblack VHMS deposits. Previous attempts to determine the age of the felsic volcanic host rocks in the Niblack area have resulted in conflicting results and interpretations. We have utilized chemical abrasion-isotope dilution-thermal ionization mass spectrometry (CA-ID-TIMS) U-Pb zircon geochronology to acquire highly precise crystallization and maximum depositional ages for a total of six samples of felsic volcanic and intrusive rocks from Niblack. This study establishes age constraints for the Niblack felsic succession of (1) crystallization ages of 565.1 ± 0.9 and 564.8 ± 1.0 Ma for coherent rhyolite flows, (2) maximum depositional ages of 565.3 ± 0.9 and 565.2 ± 0.9 Ma for felsic volcaniclastic rocks, (3) a crystallization age of 565.2 ± 0.9 Ma for a quartz-feldspar-phyric subvolcanic sill, and (4) a crystallization age of 564.8 ± 1.0 Ma for a felsic dike that crosscuts the Niblack felsic succession. These results indicate that the ~200-m-thick Niblack felsic succession and VHMS deposits formed during one episode of felsic volcanism at ca. 565.1 ± 0.9 Ma and are thus confirmed as part of the Neoproterozoic Wales Group. Results of this study provide the first chronostratigraphic framework for felsic volcanism associated with VHMS deposit formation at Niblack and have implications for mineral exploration on Prince of Wales Island and elsewhere in the Alexander terrane.