Designing overlap interaction adsorbents with high surface area has emerged as an intriguing method to enhance adsorption performance. Herein, a two-dimensional (2D) few-layer graphene-like boron nitride (g-BN) with 556 m(2) g(-1) surface area was successfully prepared and employed in the adsorption of aromatic organic pollutants methylene blue (MB) and rhodamine B (RhB) via pi-pi overlap interaction. The adsorption contact time, temperature, pH, kinetics, isotherms, and thermodynamics were investigated. The pseudo-second-order kinetic model fitted well with experimental data and isothermal data displayed better fit with the Freundlich model. The experimental results showed that the equilibrium adsorption capacity of g-BN for MB and RhB was high, 522 and 488 mg g(-1), respectively. The thermodynamic parameters suggested that the adsorption processes were spontaneous and exothermic. Based on the density functional theory (DFT), the adsorption mechanism was probably dominated by pi-pi stacking interaction with overlap form, which was confirmed by the XRD, FTIR, and Freundlich isotherm. These findings displayed that gBN was a desirable adsorbent for removing aromatic organic pollutants from wastewater.