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The occlusion of carbon (C) by phytoliths, the recalcitrant silicified structures deposited within plant tissues, is an important persistent C sink mechanism for croplands and other grass-dominated ecosystems. By constructing a silica content-phytolith content transfer function and calculating the magnitude of phytolith C sink in global croplands with relevant crop production data, this study investigated the present and potential of phytolith C sinks in global croplands and its contribution to the cropland C balance to understand the cropland C cycle and enhance long-term C sequestration in croplands. Our results indicate that the phytolith sink annually sequesters 26.35±10.22 Tg of carbon dioxide (CO2) and may contribute 40±18% of the global net cropland soil C sink for 1961–2100. Rice (25%), wheat (19%) and maize (23%) are the dominant contributing crop species to this phytolith C sink. Continentally, the main contributors are Asia (49%), North America (17%) and Europe (16%). The sink has tripled since 1961, mainly due to fertilizer application and irrigation. Cropland phytolith C sinks may be further enhanced by adopting cropland management practices such as optimization of cropping system and fertilization. [ABSTRACT FROM AUTHOR]