This work reports the fabrication of magnetic polymer dimers with controlled surface anisotropy. Thefabrication process involves the preparation of magnetite (Fe3O4) magnetic clusters with strong magnetism,followed by their surface modification, dispersion polymerization while using them as seeds,multilayer shell formation via layer-by-layer deposition, and polymer core swelling. The interplaybetween the swelling and multilayer shells generates pressure inside the multilayer-deposited, magneticpolystyrene (PS) spheres, forming structurally anisotropic dimers with single PS protrusions anchored onthe multilayer surfaces within minutes. The use of titania precursor and different swelling agents, alongwith the change in the composition of the multilayer shell, enables the introduction of different surfaceanisotropies, such as the surface-charge anisotropy, anisotropic hydrophilicity/hydrophobicity, andmaterial composition anisotropy, to the dimers. The strong magnetic response of the dimers, attributedto the magnetic cluster seeds, in combination with the surface-charge and material composition anisotropiesallows a rapid magnetic recovery and an excellent reusability, enabling their application to 20-cycled reduction of 4-nitrophenol (4-NP) and methylene blue (MB) without loss of catalytic activity. Furthermore, the anisotropic hydrophilicity/hydrophobicity makes the dimers potentially useful as solidsurfactant to stabilize immiscible oil–water mixture.