The existence of unusually large fluctuations in the Neoproterozoic (1,000-543 million years ago) carbon-isotopic record implies strong perturbations to the Earth's carbon cycle. To analyze these fluctuations, we examine records of both the isotopic content of carbonate carbon and the fractionation between carbonate and marine organic carbon. Together, these are inconsistent with conventional, steady-state models of the carbon cycle. The records can be well understood, however, as deriving from the nonsteady dynamics of two reactive pools of carbon. The lack of a steady state is traced to an unusually large oceanic reservoir of organic carbon. We suggest that the most significant of the Neoproterozoic negative carbon-isotopic excursions resulted from increased remineralization of this reservoir. The terminal event, at the Proterozoic-Cambrian boundary, signals the final diminution of the reservoir, a process that was likely initiated by evolutionary innovations that increased export of organic matter to the deep sea.