Oxygen reduction reaction (ORR) is of critical significance in the advancement of fuel cells and zinc-air batteries. The iron-nitrogen (Fe−N_x) sites exhibited exceptional reactivity towards ORR. However, the task of designing and controlling the local structure of Fe species for high ORR activity and stability remains a challenge. Herein, we have achieved successful immobilization of Fe species onto the highly curved surface of S, N co-doped carbonaceous nanosprings (denoted as FeNS/Fe₃C@CNS). The induction of this twisted configuration within FeNS/Fe₃C@CNS arose from the assembly of chiral templates. For electrocatalytic ORR tests, FeNS/Fe₃C@CNS exhibits a half-wave potential (E_1/2) of 0.91 V in alkaline medium and a E_1/2 of 0.78 V in acidic medium. The Fe single atoms and Fe₃C nanoparticles are coexistent and play as active centers within FeNS/Fe₃C@CNS. The highly curved surface, coupled with S substitution in the coordination layer, served to reduce the energy barrier for ORR, thereby enhancing the intrinsic catalytic activity of the Fe single-atom sites. We also assembled a wearable flexible Zn-air battery using FeNS/Fe₃C@CNS as electrocatalysts. This work provides new insights into the construction of highly curved surfaces within carbon materials, offering high electrocatalytic efficacy and remarkable performance for flexible energy conversion devices.