Recent drilling of continuous cores in southernmost Florida has documented a thick unit of upper Neogene siliciclastics subjacent to surficial shallow-water Quaternary carbonates exposed on islands of the Florida Keys. The siliciclastics comprise the Long Key Formation and were identified in two cores collected from the middle and upper Florida Keys. A chronologic model based on new planktic foraminiferal biochronology and strontium-isotope chronology suggests the timing of siliciclastic deposition and provides a basis for regional correlation. The chronologic model, supplemented by vertical trends in quartz grain size, pattern of planktic menardiiform coiling direction, and paleoenvironmental interpretations of benthic foraminiferal assemblages, shows that the Long Key Formation contains three intervals (I-III) of varying thickness, grain-size composition, and paleowater depth. Interval I is uppermost Miocene. The quartz grains in Interval I fine upward from basal very coarse sand to fine and very fine sand. Benthic foraminifera indicate an upward shift from an outer-shelf to inner-shelf depositional environment. Interval II, deposited during the late early to early late Pliocene, contains reworked upper Miocene siliciclastics and faunas. In the upper Keys, quartz grains in Interval II range from very coarse sand that fines upward to very fine sand and then coarsens to very coarse and medium sand. In situ benthic faunas indicate an upward shift from outer-shelf to inner-shelf deposition. In the middle Keys, Interval II is different, with the quartz grains ranging primarily from medium to very fine sand. In situ benthic taxa indicate deposition on an inner shelf. In both the middle and upper Keys, the upper Pliocene siliciclastics of Interval III contain quartz grains ranging from very coarse to very fine sands that were deposited on an inner shelf. A sequence boundary between Interval I and Interval II is suggested by; an abrupt shift in the strontium-isotope chemostratigraphy; coarsening in quartz grain size above the boundary; an abrupt landward shift in depositional facies in the upper Keys core; and a distinct variation in the predominant coiling direction of the menardiiform planktic foraminifera, from fluctuating dextral-sinistral to dextral in the upper Keys core. Successive siliciclastic infilling, likely associated with eustatic sea-level change and current redeposition, formed a foundation for subsequent carbonate deposition. Deep-sea biostratigraphic techniques, integrated with ages derived from strontium-isotope chemostratigraphy, can be successfully applied to coastal-margin sequences, even though a depauperate suite of faunal markers is common.