Galvanodynamic synthesis is introduced as a new flexible electrochemical method for the preparation of electroactive materials, as utilized for electropolymerization of aniline in the present seminal work. It is indeed a missing method in the four possible electrochemical methods namely potentiodynamic, potentiostatic, galvanostatic, and finally galvanodynamic. This explicit comparative study shows the flexibility of this method in controlling the physical and electrochemical properties of the polyaniline film. Electrochemical polymerization was performed by scanning the current in a given range. Different approaches for this purpose were also introduced as the synthesis can be performed under different conditions through linear scanning, cyclic scanning, and repetitive cyclic scanning. Effects of various controllable parameters, such as scan rate, the current range, and the scan direction were also examined. In comparison with other electrochemical methods, galvanodynamic synthesis has higher flexibility to alter controllable parameters in favor of a specific application. For instance, synthesis of polyaniline to display characteristic redox peaks suitable for battery performance or strong capacitive behavior ideal for supercapacitors.