Chert, porcelainite, and other siliceous phases are exceptionally common in Atlantic sedimentary records of the early Eocene, but the origins of these facies remain enigmatic. The early Eocene was also the warmest interval of the entire Cenozoic Era, punctuated by numerous discrete warming events termed "hyperthermals," the largest of which is termed the Paleocene-Eocene Thermal Maximum (similar to 56 Ma). Here we present new and published lithologic and carbon isotope records of silica-bearing lower Eocene sediments and suggest a link between the ubiquitous Atlantic cherts of that time period and hyperthermal events. Our data demonstrate that many of these Atlantic siliceous horizons coincide with negative carbon isotope excursions (a hallmark of hyperthermal events), including a previously unrecognized record of the Paleocene-Eocene Thermal Maximum in the South Atlantic. Hyperthermal-associated silica burial appears to be focused in the western middle to high latitudes of both the North and South Atlantic, with no association between siliceous facies and hyperthermal events found in the Pacific. We also present a new model of the coupled carbon and silica cycles (LOSiCAR) to demonstrate that enhanced silicate weathering during these events would require a rapid increase in total marine silica burial. Model experiments that include previously suggested transient reversals in the pattern of deep-ocean circulation during hyperthermals demonstrate that such a mechanism can explain the apparent focusing of elevated silica burial into the Atlantic. This combination-a silicate weathering feedback in response to global warming along with a circulation-driven focusing of silica burial-represents a new mechanism for the formation of deep-sea cherts in lower Eocene Atlantic sedimentary records and may be relevant to understanding chert formation in other intervals of Earth history.