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Effective pollutant removal with environmentally friendly materials has attracted considerable attention. Herein, macroporous polyHIPE-g-poly(glycidyl methacrylate)-β-cyclodextrin (a) was prepared via a combination of high-internal-phase emulsion (HIPE) polymerization, atom-transfer radical polymerization (ATRP), and ring-opening addition reaction techniques. Based on the PGMA brush, β-CD molecules were successfully grafted onto the surface of PHIPE. Characterization of the obtained material demonstrated a hierarchical porous structure and the successful grafting of β-CD. Attributed to the large surface area of the monolith and the host–guest molecular recognition between β-CD and BPA, the prepared PHIPE-g-PGMA-β-CD as a robust macroporous complex could effectively remove BPA from water. The removal efficiency was systematically investigated with varying the time and concentration. Moreover, the monolith could be reused by simply leaching and washing in methanol to elute BPA, displaying comparative regeneration efficiency after six cycles. The newly fabricated macroporous PHIPE-g-PGMA-β-CD has great potential application in BPA-contaminated water treatment and environmental protection. [ABSTRACT FROM AUTHOR]