Manure biogas residue has attracted increasing attention in waste recycling but faces substantial challenges because of its low carbon content, high ash content, and high heavy metal content. A novel sequential carbonization approach was proposed for recycling biogas residue; this approach consisted of pre-pyrolysis, activation with Ca(OH)2, and then activation with KOH. Pig manure-derived biogas residue was upcycled into engineered biochar (EB) with a high yield (26 %) and showed excellent performance in removing a typical plasticizer, diethyl phthalate (DEP). The proportion of carbon content greatly increased from 18 % (biogas residue) to 67 % (EB); however, the ash content decreased from 50 % (biogas residue) to 24 % (EB). The concentration of heavy metals decreased, and Zn had the largest decrease from 713 mg kg−1 to 61 mg kg−1 (p < 0.001). The sorption of DEP onto EB was rapid and reached equilibrium within 20 h. The developed specific surface area of EB was 1247 m2/g and provided abundant sorption sites for DEP; additionally, the sorption quantity reached 309 mg/g. The sorption capacity was dominated by surface adsorption. The oxygen-containing functional groups, graphene structure, porous structure, and hydrophobicity of EB contributed to the pore filling, hydrogen bonding, π–π stacking, and partitioning processes. Furthermore, the EB showed excellent practical application potential and great cycling stability. A sequential carbonization strategy was proposed to upcycle manure biogas residue into the EB for DEP removal; moreover, this strategy can aid in the attainment of environmental sustainability, including sustainable waste management and environmental pollution mitigation.