Grain legumes and drylands cereals including chickpea (Cicer arietinum), common bean (Phaseolus vulgaris), cowpea (Vigna unguiculata), groundnut (Arachis hypogaea), lentil (Lens culinaris), pigeon pea (Cajanus cajan), soybean (Glycine max), finger millet (Eleusine coracana), pearl millet (Pennisetum glaucum) and sorghum (Sorghum bicolor) are the leading sources of food grain in drylands of Africa and South Asia. These crops can help smallholder agriculture to become more resilient, productive, and profitable, but their quantitative impact on carbon sequestration is unknown. The aim of this review study was to quantify their contribution to carbon sequestration across the drylands of Africa and South Asia based on 437 publications with 1319 observations in studies conducted across 32 countries. Cropping systems with grain legumes showed the greatest increase in soil organic carbon (SOC) concentrations, while cereals (and pigeon pea) gave the largest amount of aboveground carbon stock (>2 Mg C ha−1). Estimated carbon stock in post-harvest residues of these crops was 1.51 ± 0.05 Mg C ha−1 in Africa and 2.29 ± 0.10 Mg C ha−1 in South Asia. These crops produced more aboveground carbon, and significantly increased SOC, when grown as intercrops. Soils with low initial SOC (<1%) and high clay content (>32%) showed the greatest potential for carbon sequestration when cropped with grain legumes and dryland cereals. This study is the first of its kind to provide evidence that grain legumes and drylands cereals improve carbon sequestration across Africa and South Asia.