Dynamic control of the optical properties of gold nanostructures is crucial for advancing photonics technologies spanning optical signal processing, on-chip light sources and optical computing. Despite recent advances in tunable plasmons in gold nanostructures, most studies are limited to the linear or static regime, leaving the dynamic manipulation of nonlinear optical properties unexplored. This study demonstrates the voltage-controlled Kerr nonlinear optical response of gold nanofilms via the electrothermal effect. By applying relatively low voltages (~10 V), the nonlinear absorption coefficient and refractive index are reduced by 40.4% and 33.1%, respectively, due to the increased damping coefficient of gold nanofilm. Furthermore, a voltage-controlled all-fiber gold nanofilm saturable absorber is fabricated and used in mode-locked fiber lasers, enabling reversible wavelength-tuning and operation regimes switching (e.g., mode-locking—Q-switched mode-locking). These findings advance the understanding of electrically controlled nonlinear optical responses in gold nanofilms and offer a flexible approach for controlling fiber laser operations.