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This work developed a super-high performance of engineering carbonaceous adsorbents from waste banana-peel via an optimized KOH-impregnated approach, which affords outstanding structural property (SBET = 3746.5 m2 g−1, Vtotal = 2.50 cm3 g−1), far outperforming KOH-grinding method-induced counterpart and other known banana peel-derived those. Thereby, this triggers a record-high capture value of volatile organic compounds (VOCs) specific to benzene (27.55 mmol g−1) and toluene (23.82 mmol g−1) in the all known results. The structural expression characters were accurately correlated with excellent adsorption efficiency of VOCs by investigating the synthetic factor-controlling comparative samples. Ulteriorly, the adsorption selectivity prediction at different relative humidity was demonstrated through the DIH (difference of the isosteric heats), highlighting the good superiority in selective adsorption of toluene compared to benzene even under humid atmosphere. Our findings provide the possibility for the practical application and fabrication of waste biomass (banana peel)-derived functional biochar adsorbent in the environmental treatment of threatening VOCs pollutants.