In this work, very efficient VOCs adsorbent was developed from waste bovine bone. After pyrolysis at 450 °C, the bone char was treated by HPO for surface modification and activated by KCO respectively. The prepared materials were characterized by N adsorption isotherms, SEM, FT-IR, and XPS. Adsorption/desorption and regeneration behavior of VOCs were also studied. Results showed that HPO modification can effectively accelerate the adsorption process and after KCO activation, a new hierarchical pore structure was found with an ultrahigh total pore volume of 2.807 cm/g. The specific adsorption capacity for typical VOC reached ∼13.03 mmol/g which is much higher than literature data under the same condition. Static toluene adsorption test on the prepared activated bone-char revealed that the hierarchical structure has provided abundant adsorption sites and the adsorption behavior can be well described by the pseudo-second-order model. The dynamic/static adsorption ratio increased from 70.31% to 78.62% due to less mass transfer resistance by surface modification.Copyright © 2020 Elsevier Ltd. All rights reserved.