This study demonstrates the formation of biocompatible magnetic particles into organized structures upon the application of an external magnetic field. The capability to create the structures was examined in silicone-oil suspensions and in a gelatine solution, which is commonly used as a blood plasma expander. Firstly, the carbonyl iron particles were successfully coated with gelatine, mixed with a liquid medium in order to form a magnetorheological suspension, and subsequently the possibility of controlling their rheological parameters via a magnetic field was observed using a rotational rheometer with an external magnetic cell. Scanning electron microscopy, infrared spectroscopy, and thermogravimetric analysis confirmed the successful coating process. The prepared magnetorheological suspensions exhibited a transition from pseudoplastic to Bingham behavior, which confirms their capability to create chain-like structures upon application of a magnetic field, which thus prevents the liquid medium from flowing. The observed dynamic yield stresses were calculated using Robertson–Stiff model, which fit the flow curves of the prepared magnetorheological suspensions well.