Shallow soils (i.e., Lithic Entisols) cover about 20% of Brazilian drylands. Inherent soil characteristics (i.e., shallow depths) and water scarcity restrict plant growth and carbon (C) inputs in these soils. In such a sensitive ecosystem, sustainable land management options are key to promoting socio-economic development and ensuring food security. Here, we use a dataset of 50 Lithic Entisol profiles distributed within the Brazilian drylands (northeastern region) to: (i) investigate the effects of land-use (cropland, grassland, and native forest), climate (semi-arid and dry sub-humid), and slope classes (0–3%, 3–8%, 8–20% and 20–45%) on soil C accumulation; and (ii) evaluate how understanding multiple drivers C accumulation can support the identification of sustainable land management options. The results suggested that land use does not affect C stock and C/N ratio, nevertheless, they were affected by climate. Under dry sub-humid climate conditions, C stocks were 41.7 Mg ha−1, 44% higher than under semi-arid climate (28.9 Mg ha−1), a result that reflects the effect of higher biomass production in wetter environments. Under slopes of 20–45%, C stocks were 54.3 Mg ha−1, 172% higher than under slopes of 0–3% (19.9 Mg ha−1), because of the higher altitudes and wetter conditions under steeper slopes. Our results showed that areas under lower slopes have lower C stocks and lower aridity index. These drier conditions reduce the productive potential of annual crops and grasslands but enable the cultivation of high-yielding Crassulacean Acid Metabolism (CAM) crops, such as Agave spp, which have a high potential for biofuel production. Furthermore, the possibility of reintroducing organic residues from ethanol production can promote an increase in C stocks, contributing to climate change mitigation. Ultimately, our study provides insights from a holistic view of SOC accumulation drivers, supporting land use planning of highly sensitive environments in tropical drylands around the world.