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Spheroidal beads present an exterior surface of a hydrophilic permeable, deformable hydrogel, which is an isocyanate-functional polymer that is polymerized by urethane bonds and cross-linked by urethane and urea bonds. Sequestering agents at or near the surface are covalently bound to isocyanate groups or to intermediate linkers that are so bound, and the deformable hydrogel allows sequestering agents to retain their native three-dimensional configurations. As a result of such hydrogel characteristics and hydrophilicity, the beads achieve highly effective capture of very small subpopulations of rare cells from bodily fluids or the like and very effectively deter nonspecific binding of other biomaterials present in such bodily fluid. They may be all-hydrogel spheroids or hydrogel-coated substrates.