To address the challenges of high energy consumption and low efficiency in recovering phenols and oils from coal chemical wastewater (CCW), this study focused on the design and synthesis of metal–organic frameworks and spherical carbon particle (MOFs/SCP) adsorbents with a high adsorption capacity and ease of desorption. Additionally, a new comprehensive treatment mode named “adsorption-desorption-regeneration-recovery” (ADRR) was developed to efficiently recover phenols and oils from CCW. The results revealed that the ADRR treatment mode maintained high adsorption and desorption efficiencies of MOFs/SCP, which remained consistently above 95 %. Additionally, methanol regeneration reached ∼ 90 %, and the recovery efficiency of phenols and oils was ∼ 83 %. The analysis of the adsorption behavior model indicated that the adsorption of phenols and oils by MOFs/SCP mainly involved monolayer chemical adsorption characterized by spontaneity, heat absorption, and disorder. The dynamic adsorption model exhibited a strong correlative ability to predict and assess the adsorption capacity, rate, equilibrium, and operating parameters. Finally, structural analyses and molecular dynamics simulations revealed that the micro-interaction mechanisms between MOFs/SCP and phenols and oils mainly depended on the distinctive hydrophobic nature and porous adsorption capabilities of MOFs/SCP. These interactions were mainly facilitated by electrostatic interactions, π–π interactions, and hydrogen bonding. The findings of the study are crucial for achieving high-value recovery of phenols and oils from CCW and, promoting the clean and sustainable growth of the coal chemical industry.