Rationally designed defects in a crystal can confer unique properties. This study showcases a novel dual‐defects engineering strategy to tailor the electrochemical response of metal‐organic framework (MOF) materials used for electrochemical energy storage. We identify salicylic acid (SA) as an effective modulator to control MOF‐74 growth and induce structural defects, and adopt cobalt cation doping for introducing a second type of defect. The resulting dual‐defects engineered bimetallic MOF exhibits a discharging capacity of 218.6 mAh/g — 4.4 times that of the pristine MOF‐74— and significantly improved cycling stability. Moreover, the engineered MOF‐74(Ni0.675Co0.325)‐8//Zn aqueous battery showed top energy/power density performances for Ni‐Zn batteries (266.5 Wh/kg, 17.22 kW/kg). Comprehensive investigations reveal that engineered defects modify the local coordination environment and promote the in‐situ electrochemical reconfiguration during operation to significantly boost the electrochemical activity. This work suggests that rational tailoring the defects within the MOF crystal is an effective strategy to manipulate the coordination environment of the metal centers and the corresponding electrochemical reconfiguration for electrochemical applications.This article is protected by copyright. All rights reserved