This study introduces an electrochemical doping strategy to manipulate the structure and composition of electrically conductive metal-organic frameworks (c-MOFs). The research focuses on a representative c-MOF, Ni₃(HITP)₂, synthesized into porous thin films supported by nanocellulose. The c-MOF exhibits capacitive behavior in neutral electrolyte and redox behavior in both acidic and alkaline electrolytes. The organic ligands within the c-MOF undergo oxidation (p-doping) and reduction (n-doping) when exposed to specific electrochemical potentials in acidic and alkaline electrolytes, respectively. The p-doping process is reversible, while the n-doping is irreversible, leading to the gradual decomposition of the framework into inorganic species. The study demonstrates the versatile electrochemical applications of c-MOFs, including electrochemical energy storage, electrocatalysis, and ultrafast actuation. The findings provide profound insights into the doping of c-MOFs, offering a new avenue for modulating their chemical and electronic structure, thereby broadening their potential for diverse electrochemical applications. The electrochemical behavior of c-MOFs is strongly dependent on the pH of the electrolyte, allowing for the development of proof-of-concept applications in various scenarios. These applications include electrochemical energy storage in acidic electrolytes, actuation in neutral electrolytes, and electrocatalytic oxygen evolution in alkaline electrolytes. The study also highlights the structural stability of nanocellulose under electrochemical conditions and the potential of c-MOFs as efficient and stable electrochemical catalysts. The research provides a novel approach to manipulate the structure and composition of c-MOFs, opening avenues for exploring new applications in diverse fields such as new electronic devices, sensing, and catalysis.This study introduces an electrochemical doping strategy to manipulate the structure and composition of electrically conductive metal-organic frameworks (c-MOFs). The research focuses on a representative c-MOF, Ni₃(HITP)₂, synthesized into porous thin films supported by nanocellulose. The c-MOF exhibits capacitive behavior in neutral electrolyte and redox behavior in both acidic and alkaline electrolytes. The organic ligands within the c-MOF undergo oxidation (p-doping) and reduction (n-doping) when exposed to specific electrochemical potentials in acidic and alkaline electrolytes, respectively. The p-doping process is reversible, while the n-doping is irreversible, leading to the gradual decomposition of the framework into inorganic species. The study demonstrates the versatile electrochemical applications of c-MOFs, including electrochemical energy storage, electrocatalysis, and ultrafast actuation. The findings provide profound insights into the doping of c-MOFs, offering a new avenue for modulating their chemical and electronic structure, thereby broadening their potential for diverse electrochemical applications. The electrochemical behavior of c-MOFs is strongly dependent on the pH of the electrolyte, allowing for the development of proof-of-concept applications in various scenarios. These applications include electrochemical energy storage in acidic electrolytes, actuation in neutral electrolytes, and electrocatalytic oxygen evolution in alkaline electrolytes. The study also highlights the structural stability of nanocellulose under electrochemical conditions and the potential of c-MOFs as efficient and stable electrochemical catalysts. The research provides a novel approach to manipulate the structure and composition of c-MOFs, opening avenues for exploring new applications in diverse fields such as new electronic devices, sensing, and catalysis.