Laser-scribed graphene electrodes (LSGEs) have attracted great attention for the development of electrochemical (bio)sensors due to their excellent electronic properties, large surface area, and high porosity, which enhances the electrons' transfer rate. An increasing active surface area and defect sites are the quickest way to amplify the electrochemical sensing attributes of the electrodes. Here, we have found that the activation procedure coupled to the electrodeposition of metal nanoparticles resulted in a significant amplification of the active area and the analytical performance. This preliminary study is supported by the demonstration of the simultaneous electrochemical sensing of dopamine (DA) and uric acid (UA) by the electrochemically activated LSGEs (LSGE*s). Furthermore, the electrodeposition of two different metal nanoparticles, gold (Au) and silver (Ag), was performed in multiple combinations on working and reference electrodes to investigate the enhancement in the electrochemical response of LSGE*s. Current enhancements of 32, 27, and 35% were observed from LSGE* with WE:Au/RE:LSG/CE:LSGE, WE:Au/RE:Au/CE:LSGE, and WE:Au/RE:Ag/CE:LSGE, compared to the same combinations of LSGEs without any surface activation. A homemade and practical potentiostat, KAUSTat, was used in these electrochemical depositions in this study. Among all of the combinations, the surface area was increased 1.6-, 2.0-, and 1.2-fold for WE:Au/RE:LSG/CE:LSGE, WE:Au/RE:Au/CE:LSGE, and WE:Au/RE:Ag/CE:LSGE prepared from LSGE*s, respectively. To evaluate the analytical performance, DA and UA were detected simultaneously in the presence of ascorbic acid. The LODs of DA and UA are calculated to be ∼0.8 and ∼0.6 μM, respectively. Hence, this study has the potential to open new insights into new surface activation strategies with a combination of one-step nanostructured metal depositions by a custom-made potentiostat. This novel strategy could be an excellent and straightforward method to enhance the electrochemical transducer sensitivity for various electrochemical sensing applications.