Pulse ionized titania 3D-nanonetworks (T3DN) are emerging materials for fabricating binder-free and carbon-free electrodes for electrochemical energy storage devices. In this article, we investigate the effect of the one of the most important fabrication parameters, pulse frequency, for optimizing supercapacitor efficiency. A series of coin cell batteries with laser-induced electrodes was fabricated; the effect of pulse frequency on oxidation levels and material properties was studied using both experimental and theoretical analysis. Also, detailed electrochemical tests including cyclic voltammetry (CV), charge/discharge, and electrochemical impedance spectroscopy (EIS) were conducted to better understand the effect of pulse frequency on the electrochemical performance of the fabricated devices. The results show that at a frequency of 600 kHz, more T3DN were observed due to the higher temperature and stabler formation of the plasma plume, which resulted in better performance of the fabricated supercapacitors; specific capacitances of samples fabricated at 600 kHz and 1200 kHz were calculated to be 59.85 and 54.39 mF/g at 500 mV/s, respectively.