This study presents a high-capacity and high-rate sodium-ion battery anode based on ultrathin layered tin(II) sulfide (SnS) nanostructures supported on graphene foam (GF). The SnS nanoarray anode exhibits a high reversible capacity of ~1,100 mAh g⁻¹ at 30 mA g⁻¹ and ~420 mAh g⁻¹ at 30 A g⁻¹, outperforming its lithium-ion storage performance. The high performance is attributed to the surface-dominated redox reaction enabled by the tailored ultrathin SnS nanostructures, which also work in other layered materials for high-performance sodium-ion storage. The study addresses the challenge of achieving fast charging and high power density in sodium-ion electrodes due to sluggish sodiation kinetics. The SnS nanostructures, grown via a one-step hot bath method, offer a unique combination of high electrical conductivity, high capacity, and earth abundance, making them a promising anode material for sodium-ion batteries. The SnS nanostructures exhibit a smaller lattice expansion during sodiation/desodiation compared to SnS₂, which correlates with a two-structure phase reaction in SnS compared to the three-structure transformation in SnS₂. The study demonstrates that the SnS nanostructures exhibit a significant pseudocapacitive contribution, which enhances the rate capability and capacity of the sodium-ion battery. The pseudocapacitive contribution is quantified through kinetic analysis, revealing that the NH electrode has the highest pseudocapacitive contribution (~84%) at 0.8 mV s⁻¹. The NH electrode also shows superior rate capability, with a discharge capacity of over 400 mAh g⁻¹ at 30 A g⁻¹, which is higher than that of the Li⁺ electrode. The study compares the performance of SnS NH anode for both Na⁺ and Li⁺ storage, showing that the SnS NH electrode exhibits superior rate capacity and capacitive contribution for Na⁺ storage compared to Li⁺. The results suggest that the surface-dominated extrinsic pseudocapacitance is a major energy-storage mechanism for high capacity and fast Na⁺ uptake. The study also highlights the importance of the electrode architecture in achieving high-rate charge/discharge performance, with the SnS NH electrode showing superior performance due to its few-layered architecture and mesoporous iso-oriented nanocrystals. The study concludes that the SnS nanostructures, supported on graphene foam, offer a promising solution for high-capacity and high-rate sodium-ion storage, with the potential to revolutionize sodium-ion battery technology. The results demonstrate the importance of nanoscale engineering in enhancing the performance of sodium-ion batteries, and the study provides a framework for further development of sodium-ion battery materials.This study presents a high-capacity and high-rate sodium-ion battery anode based on ultrathin layered tin(II) sulfide (SnS) nanostructures supported on graphene foam (GF). The SnS nanoarray anode exhibits a high reversible capacity of ~1,100 mAh g⁻¹ at 30 mA g⁻¹ and ~420 mAh g⁻¹ at 30 A g⁻¹, outperforming its lithium-ion storage performance. The high performance is attributed to the surface-dominated redox reaction enabled by the tailored ultrathin SnS nanostructures, which also work in other layered materials for high-performance sodium-ion storage. The study addresses the challenge of achieving fast charging and high power density in sodium-ion electrodes due to sluggish sodiation kinetics. The SnS nanostructures, grown via a one-step hot bath method, offer a unique combination of high electrical conductivity, high capacity, and earth abundance, making them a promising anode material for sodium-ion batteries. The SnS nanostructures exhibit a smaller lattice expansion during sodiation/desodiation compared to SnS₂, which correlates with a two-structure phase reaction in SnS compared to the three-structure transformation in SnS₂. The study demonstrates that the SnS nanostructures exhibit a significant pseudocapacitive contribution, which enhances the rate capability and capacity of the sodium-ion battery. The pseudocapacitive contribution is quantified through kinetic analysis, revealing that the NH electrode has the highest pseudocapacitive contribution (~84%) at 0.8 mV s⁻¹. The NH electrode also shows superior rate capability, with a discharge capacity of over 400 mAh g⁻¹ at 30 A g⁻¹, which is higher than that of the Li⁺ electrode. The study compares the performance of SnS NH anode for both Na⁺ and Li⁺ storage, showing that the SnS NH electrode exhibits superior rate capacity and capacitive contribution for Na⁺ storage compared to Li⁺. The results suggest that the surface-dominated extrinsic pseudocapacitance is a major energy-storage mechanism for high capacity and fast Na⁺ uptake. The study also highlights the importance of the electrode architecture in achieving high-rate charge/discharge performance, with the SnS NH electrode showing superior performance due to its few-layered architecture and mesoporous iso-oriented nanocrystals. The study concludes that the SnS nanostructures, supported on graphene foam, offer a promising solution for high-capacity and high-rate sodium-ion storage, with the potential to revolutionize sodium-ion battery technology. The results demonstrate the importance of nanoscale engineering in enhancing the performance of sodium-ion batteries, and the study provides a framework for further development of sodium-ion battery materials.