This study introduces an electrochemical doping strategy to manipulate the structure and composition of electrically conductive metal-organic frameworks (c-MOFs). The methodology is demonstrated using Ni3(HHTP)2, a c-MOF synthesized into porous thin films supported by nanocellulose. The c-MOF exhibits capacitive behavior in neutral electrolytes but redox behaviors in acidic and alkaline electrolytes. Oxidation (p-doping) and reduction (n-doping) of the organic ligands occur under specific electrochemical potentials in acidic and alkaline electrolytes, respectively. P-doping is reversible, maintaining the c-MOF structure, while n-doping is irreversible, leading to the gradual decomposition of the framework. The study showcases the versatile electrochemical applications of c-MOFs, including energy storage, electrocatalysis, and actuation. The findings provide insights into the doping of c-MOFs, offering new avenues for modulating their chemical and electronic structures.This study introduces an electrochemical doping strategy to manipulate the structure and composition of electrically conductive metal-organic frameworks (c-MOFs). The methodology is demonstrated using Ni3(HHTP)2, a c-MOF synthesized into porous thin films supported by nanocellulose. The c-MOF exhibits capacitive behavior in neutral electrolytes but redox behaviors in acidic and alkaline electrolytes. Oxidation (p-doping) and reduction (n-doping) of the organic ligands occur under specific electrochemical potentials in acidic and alkaline electrolytes, respectively. P-doping is reversible, maintaining the c-MOF structure, while n-doping is irreversible, leading to the gradual decomposition of the framework. The study showcases the versatile electrochemical applications of c-MOFs, including energy storage, electrocatalysis, and actuation. The findings provide insights into the doping of c-MOFs, offering new avenues for modulating their chemical and electronic structures.