A novel graphene wool (GW) material was used as adsorbent for the removal of phenanthrene (PHEN) and pyrene (PYR) from aqueous solution. Adsorption kinetics, adsorption isotherms, thermodynamics of adsorption and effect of pH, ionic strength, and temperature on the adsorption of PHEN and PYR onto GW were comprehensively investigated. Isothermal and kinetic experimental data were fit to Langmuir, Freundlich, Temkin, Sips and Dubinin–Radushkevich models, as well as pseudo-first-order and pseudo-second-order kinetic models. The adsorption kinetic data best fit the pseudo-second-order kinetic model for PHEN and PYR sorption with R2 value >0.999, whilst the Sips model best fit isotherm data. Kinetic data revealed that 24 hr of contact between adsorbent and polycyclic aromatic hydrocarbons (PAHs) was sufficient for maximum adsorption, where the Langmuir maximum adsorption capacity of GW for PHEN and PYR was 5 and 20 mg g−1 and the optimum removal efficiency was 99.9% and 99.1%, respectively. Thermodynamic experiments revealed that adsorption processes were endothermic and spontaneous. Desorption experiments indicated that irreversible sorption occurred with a hysteresis index greater that zero for both PAHs. The high adsorption capacity and potential reusability of GW makes it a very attractive material for removal of hydrophobic organic micro-pollutants from water.