We applied tandem U-Pb dating of detrital zircon (DZ) to redefine the Tonto Group in the Grand Canyon region (Arizona, USA) and to modify the Cambrian time scale. Maximum depositional ages (MDAs) based upon youngest isotope-dilution DZ ages for the Tapeats Sandstone are ≤508.19 ± 0.39 Ma in eastern Grand Canyon, ≤507.68 ± 0.36 Ma in Nevada, and ≤506.64 ± 0.32 Ma in central Arizona. The Sixtymile Formation, locally conformable below the Tapeats Sandstone, has a similar MDA (≤508.6 ± 0.8 Ma) and is here added to the Tonto Group. We combined these precise MDAs with biostratigraphy of trilobite biozones in the Tonto Group. The Tapeats Sandstone is ca. 508–507 Ma; the Bright Angel Formation contains Olenellus, Glossopleura, and Ehmaniella biozones and is ca. 507–502 Ma; and the Muav Formation contains Bolaspidella and Cedaria biozones and is ca. 502–499 Ma. The Frenchman Mountain Dolostone is conformable above the Muav Formation and part of the same transgression; it replaces McKee’s Undifferentiated Dolomite as part of the Tonto Group; it contains the Crepicephalus Biozone and is 498–497 Ma. The Tonto Group thickens east to west, from 250 m to 830 m, due to ∼300 m of westward thickening of carbonates plus ∼300 m of eastward beveling beneath the sub-Devonian disconformity. The trilobite genus Olenellus occurs in western but not eastern Grand Canyon; it has its last appearance datum (LAD) in the Bright Angel Formation ∼45 m above the ≤507.68 Ma horizon. This extinction event is estimated to be ca. 506.5 Ma and is two biozones below the Series 2–Miaolingian Epoch boundary, which we estimate to be ca. 506 Ma. Continued tandem dating of detrital grains in stratigraphic context, combined with trilobite biostratigraphy, offers rich potential to recalibrate the tempo and dynamics of Cambrian Earth systems.