<p>Limited by low conductivity, designing cathode materials with excellent electron transfer efficiency for high-performance nickel-zinc batteries (NZBs) remains challenging. In this study, a series of bimetallic metal-organic nanowires were fabricated by doping M ions in NiNTA, resulting in NiMNTA (M = Mg²⁺, Mn²⁺, Co²⁺, Zn²⁺, Ag⁺), and Ni_<i>x</i>Co_6−<i>x</i>NTA (<i>x</i> = 1, 2, 3, 4, 5). The proportions and types of metal ions can be modified without altering the initial coordination structure. X-ray absorption fine structure spectroscopy (XAFS) revealed that only M–O bonds, not metal bonds, were present in the material. The performance of Ni₂Co₄NTA as the cathode for aqueous NZBs was significantly improved, achieving the maximum energy density of 279.17 Wh kg⁻¹ with the high cycle stability (retention rate of 72.0% after 1,000 cycles). The flexible Ni₂Co₄NTA//Zn@carbon cloth battery employing gel electrolyte also exhibits the excellent Coulombic efficiency of 96% after 350 cycles. This approach shows considerable potential for designing one-dimensional materials with bimetallic modifications, providing new strategies for developing cathode materials for NZBs with high specific capacity and cycle stability.</p>