The study is a first-time investigation into the use of Eucalyptus leaves as a low-cost herbal adsorbent for the removal of arsenic (As) and mercury (Hg) from aqueous solutions. The adsorption capacity and efficiency were studied under various operating conditions within the framework of response surface methodology (RSM) by implementing a four-factor, five-level Box-Wilson central composite design (CCD). A pH range of 3-9, contact time (t) of 5-90 min, initial heavy metal (As or Hg) concentration (C0) of 0.5-3.875 mg/L, and adsorbent dose (m) of 0.5-2.5 g/L were studied for the optimization and modeling of the process. The adsorption mechanism and the relevant characteristic parameters were investigated by four two-parameter (Langmuir, Freundlich, Temkin, and Dubinin-Radushkevich) isotherm models and four kinetic models (Lagergren's pseudo-first order (PFO), Ho and McKay's pseudo-second order (PSO), WeberMorris intraparticle diffusion, and modified Freundlich). The new nonlinear regression-based empirical equations, which were derived within the scope of the study, showed that it might be possible to obtain a removal efficiency for As and Hg above 94% at the optimum conditions of the present process-related variables (pH = 6.0, t = 47.5 min, C0 = 2.75 mg/L, and m = 1.5 mg/L). Based on the Langmuir isotherm model, the maximum adsorption or uptake capacity of As and Hg was determined as 84.03 and 129.87 mg/g, respectively. The results of the kinetic modeling indicated that the adsorption kinetics of As and Hg were very well described by Lagergren's PFO kinetic model (R2 = 0.978) and the modified Freundlich kinetic model (R2 = 0.984), respectively. The findings of this study clearly concluded that the Persian Eucalyptus leaves demonstrated a higher performance compared to several other reported adsorbents used for the removal of heavy metals from the aqueous environment.