Featured Application: Alginate-based ferrogels and magneto-rheological suspensions are advanced materials for biomedical and bioengineering applications as scaffolds for cell proliferation, targeted drug delivery, templates for tissue regeneration and engineering. Alginate gels are extensively tested in biomedical applications for tissue regeneration and engineering. In this regard, the modification of alginate gels and solutions with dispersed magnetic particles gives extra options to control the rheo-elastic properties both for the fluidic and gel forms of alginate. Rheological properties of magnetic suspensions based on Na-alginate water solution with embedded magnetic particles were studied with respect to the interfacial adhesion of alginate polymer to the surface of particles. Particles of magnetite (Fe3O4), metallic iron (Fe), metallic nickel (Ni), and metallic nickel with a deposited carbon layer (Ni@C) were taken into consideration. Storage modulus, loss modulus, and the shift angle between the stress and the strain were characterized by the dynamic mechanical analysis in the oscillatory mode. The intensity of molecular interactions between alginate and the surface of the particles was characterized by the enthalpy of adhesion which was determined from calorimetric measurements using a thermodynamic cycle. Strong interaction at the surface of the particles resulted in the dominance of the “fluidic” rheological properties: the prevalence of the loss modulus over the storage modulus and the high value of the shift angle. Meanwhile, poor interaction of alginate polymer with the surface of the embedded particles favored the “elastic” gel-like properties with the dominance of the storage modulus over the loss modulus and low values of the shift angle.