Carbonaceous adsorbents were synthesized from palm kernel shell and palm mesocarp fiber for the adsorption of phenanthrene (PHE) and the highly carcinogenic-benzo(a)pyrene (BaP). The structure and properties of the activated biochar were characterized using standardized analytical tools. The microscopic examinations carried out with SEM and BET results revealed mesoporous structures and interstitial spaces in the activated samples (AB-PKS and AB-PMS). Powder X-ray diffraction (PXRD) results showed that prepared sorbents are amorphous and that activation affected the amorphous cellulose on the surface of the microfibrils which led to a decrease in the intensity of some peaks. Fourier-transform infrared spectroscopy (FTIR) affirms the availability of surface moieties that may promote polycyclic aromatic hydrocarbon (PAH) removal or decontamination of aqueous media. The sorption isotherm and effect of pH on the adsorption of PHE and BaP onto the activated palm kernel shell (AB-PKS) and activated palm mesocarp fiber (AB-PMF) were investigated. The isotherm studies and error analysis (SSE and R2) confirm that the Freundlich model best fits experimental results for AB-PMF; while, the Langmuir model best describes AB-PKS sorption of BaP and PHE, respectively. The optimal removal efficiency for PHE was between 84 and 100% while that of BaP was between 68 and 87% with maximum adsorption capacity (qmax) of 19.38–21.98 mg/g and 1.24–13.26 mg/g, respectively. The optimum pH condition for removing PHE is less than 7 and above 7 for BaP. Therefore, the conversion of waste materials to useful sorbents, as well as preliminary adsorption test results obtained suggests a cleaner and cost-effective pathway for waste management and water treatment.