Amylose is carbohydrate polymer defined as a linear natural polysaccharide composed of α(1→4) bound glucose units. Due to its abundance, renewable nature, low cost, and biodegradability, this polymer is regarded as a promising green material for producing crystals and particles of different sizes ranging from the nanometer scale to the micrometer scale. Herein, short amylose chains and dextran-coated iron oxide magnetic nanoparticles (Dex@MNPs) were introduced to fabricate individual superparamagnetic amylose microparticles (SAMPs), which have a well-defined spherical shape and a uniform size of about 1 μm. We found that the aggregation of SAMPs can be mediated by the introduced Dex@MNPs in a concentration-dependent manner, indicating that Dex@MNPs, as the seed crystals, play an important role in self-assembly of SAMPs. By using streptococcal protein G tagged with maltose binding protein (MBP-SPG), specific antibody against Escherichia coli O157:H7 was successfully immobilized on the surface of SAMPs. The Ab-functionalized SAMPs showed a high capture efficiency (>90%) comparable to the commercial immunomagnetic microparticles regardless of suspending agents (1X PBS and milk). Moreover, SAMPs exhibited excellent recyclability, in which the Ab immobilized on the surface of SAMPs can be refreshed by using the maltose elution buffer along with the unchanged capture efficiency. In addition, SAMPs were assembled into the linear rod-shape microstructure by the introduced magnetic field during the amylose-mediated precipitation process. The convenient self-assembly of SAMPs with the well-defined size and shape, biocompatibility, tolerance to environmental variances, high magnetic response behavior, and excellent recyclability in the functionalization make these magnetic microparticles promising for many potential applications such as bio-sensing, labeling, and smart delivery of active compounds.