Tainting of waterbodies with noxious industrial waste is the gravest environmental concern of the day that continues to wreak inevitable havoc on human health. To cleanup these hard-to-remove life-threatening water contaminants, we have prepared hierarchically porous poly(acrylic acid) beads by emulsion templating. These emulsion-templated macroporous polymer beads not only mediate the synthesis of Fe3O4 nanoparticles inside their porous network using a coprecipitation approach but, in turn, create diverse anchoring sites to immobilize an additional poly(acrylic acid) active layer onto the nanocomposite beads. These post-synthetically modified nanocomposite beads with macropores and abundant acrylic acid moieties offer the ready mass transfer and fair advantage of relatively higher overall negative charge to efficiently adsorb lead [Pb(II)] and crystal violet with impressive performance-even superior to many of the materials explored in this regard so far. Furthermore, the strong entanglement of nanoparticles in the porous polymeric scaffolds tackles the curb of trade-off between all-round effective remediation and secondary pollution and the millimeter size eases their processing and recovery during the adsorption tests, thereby making these materials practically worthwhile.