The increasing demand for portable and wearable electronics has promoted the development of safe and flexible yarn–based batteries with outstanding electrochemical properties. However, achieving superior energy storage performance with a high active material (AM) load and long cycle life with this device format remains a challenge. In this study, a stable and rechargeable high–performance aqueous Ni–Fe yarn battery was constructed via biscrolling to embed AMs within helical carbon nanotube (CNT) yarn corridors. Owing to the high load of charge storage nanoparticles (NPs; above 97 wt%) and the outer neat CNT layer, the buffered biscrolled Ni–Fe yarn battery demonstrates excellent linear capacity (0.053 mAh/cm) and cycling stability (60.1% retention after 300 charge/discharge cycles) in an aqueous electrolyte. Moreover, our flexible yarn battery exhibits maximum energy/power densities of 422 mWh/cm3 and 7535 mW/cm3 based on the total volume of the cathode and anode, respectively, which exceed those reported for many flexible Ni–Fe batteries. Thus, biscrolled Ni–Fe yarn batteries are promising candidates for next–generation conformal energy solutions.