Buran-Kaya III is a rockshelter located in Crimea (Ukraine). It provides an exceptional stratigraphic sequence extending from the Middle Paleolithic to the Neolithic. Nine Paleolithic layers have been attributed to the Streletskaya or eastern Szeletian, Micoquian, Aurignacian, Gravettian, and Swiderian cultural traditions. Human remains from the richest Gravettian layer (6-1) are radiocarbon dated to 31.9 ka BP, and therefore represent, with Peştera cu Oase (Romania), one of the oldest anatomically modern humans in Europe. The aim of this study is to obtain a controlled stratigraphic sequence of Buran-Kaya III with new 14C dates from faunal and human bones, in their paleoenvironmental context. During our new excavations (2009–2011), sediments, bones, and teeth from the stratigraphical layers were sampled for sedimentological, geochemical, and 14C analyses. Fossil bones from the 2001 excavations were also analyzed. Accelerator mass spectrometry (AMS) 14C dating, including cross-dating, was performed at Groningen, Saclay/Gif-sur-Yvette, and Oxford. Biogeochemical analysis was used to test the integrity of the bone collagen. Dates were modeled using a Bayesian approach. The sedimentological, paleoenvironmental, and chronological data are mutually consistent and show that the Paleolithic human occupations at Buran-Kaya III range from the end of MIS 3 to early MIS 1. These results provide a new chronological and paleoenvironmental framework for the human settlements in eastern Europe during the late Middle and the Upper Paleolithic.