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Abstract We report⁴⁰Ar‐³⁹Ar step‐heating ages of Paleocene‐Eocene (P‐E) boundary impact spherules from Atlantic Margin coastal plain and open ocean sites. We test the hypothesis that the P‐E spherules are reworked from an earlier event (e.g., K‐Pg impact at ~66 Ma), which predicts a cooling age discordant from their depositional age of 55.93 ± 0.05 Ma at the P‐E boundary. Isochrons from the step‐heating analysis yield⁴⁰Ar‐³⁶Ar intercepts in excess of the modern in most cases, indicating that the spherules have excess radiogenic Ar (⁴⁰Ar*), typical of impact glasses incompletely degassed before solidification. The weighted mean of the isochron‐corrected plateau age is 54.2 ± 2.5 Ma (1σ), and their isochron age is 55.4 ± 4.0 Ma, both indistinguishable from their P‐E depositional age, not supporting the K‐Pg reworking hypothesis. This is consistent with all other stratigraphic and geochemical evidence for an impact at the P‐E boundary and ejecta distribution by air fall.