We report the effort in designing layered SnS nanocrystals decorated on nitrogen and sulfur dual-doped graphene aerogels (SnS@N,S-GA) as anode material of SIBs. The optimized mass loading of SnS along with the addition of nitrogen and sulfur on the surface of GAs results in enhanced electrochemical performance of SnS@N,S-GA composite. In particular, the introduction of nitrogen and sulfur heteroatoms could provide more active sites and good accessibility for Na ions. Moreover, the incorporation of the stable SnS crystal structure within the anode results in the superior discharge capacity of 527 mAh g under a current density of 20 mA g upon 50 cycles. It maintains 340 mAh g even the current density is increased to 800 mA g. Aiming to further systematically study mechanism of composite with improved SIB performance, we construct the corresponding models based on experimental data and conduct first-principles calculations. The calculated results indicate the sulfur atoms doped in GAs show a strong bridging effect with the SnS nanocrystals, contributing to build robust architecture for electrode. Simultaneously, heteroatom dual doping of GAs shows the imperative function for improved electrical conductivity. Herein, first-principles calculations present a theoretical explanation for outstanding cycling properties of SnS@N,S-GA composite.