The purpose of this study was to compare the adsorption behavior of cationic and anionic dyes onto a hexagonal boron nitride (hBN) nanostructure that was rich in a negative charge. Herein, the hBN nanostructure was synthesized using boric acid as a precursor material. The characteristic peaks of the hBN nanostructure were performed using Fourier transform infrared (FT-IR) and Raman spectroscopies. The morphology and the particle size of hBN nanostructure were determined by transmission electron microscopy (TEM) and scanning electron microscopy (SEM). During the studies, various essential adsorption parameters were investigated, such as the initial dye concentration, pH of the dye solution, adsorbent dose, and contact time. Under optimal conditions, the removal of 42.6% Metanil yellow (MY) and 90% Victoria blue B (VBB) from aqueous solution was performed using a 10-mg hBN nanostructure. Furthermore, the equilibrium studies showed that the Freundlich isotherm model fitted well for the removal of MY. However, the Langmuir isotherm model fitted well for the removal of VBB. Moreover, according to the results obtained from the kinetic studies, while the first-order kinetic model was suited for the adsorption of the MY, the second-order kinetic model was found to well fit for the adsorption of VBB.