Aqueous Zn-Br batteries (ZBBs) offer promising next-generation high-density energy storage for energy storage systems, along with distinctive cost effectiveness particularly in membraneless and flowless (MLFL) form. Unfortunately, they generally suffer from uncontrolled diffusion of corrosive bromine components, which cause serious self-discharge and capacity fade. An MLFL-ZBB is presented that fundamentally tackles the problem of bromine crossover by converting bromine to the polybromide anion using protonated pyridinic nitrogen doped microporous carbon decorated on graphite felt (NGF). The NGF electrodes efficiently capture bromine and polybromide anions at the abundant protonated nitrogen dopant sites within micropores and facilitate effective conversion of bromine into polybromides through electrochemical-chemical growth mechanism. The MLFL-ZBBs with NGF exhibit an extraordinary stability over 1000 charge/discharge cycles, with an energy efficiency over 80%, the highest value ever reported among membraneless Zn-Br batteries. Judicious engineering of an atomistically designed nanostructured electrode offers a novel design platform for low cost, high voltage, long-life cycle aqueous hybrid Zn-Br batteries.