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The long-ranged interactions induced by magnetic fields and capillary forces in multiphasic fluid–particle systems facilitate the assembly of a rich variety of colloidal structures and materials. We review here the diverse structures assembled from isotropic and anisotropic particles by independently or jointly using magnetic and capillary interactions. The use of magnetic fields is one of the most efficient means of assembling and manipulating paramagnetic particles. By tuning the field strength and configuration or by changing the particle characteristics, the magnetic interactions, dynamics, and responsiveness of the assemblies can be precisely controlled. Concurrently, the capillary forces originating at the fluid–fluid interfaces can serve as means of reconfigurable binding in soft matter systems, such as Pickering emulsions, novel responsive capillary gels, and composites for 3D printing. We further discuss how magnetic forces can be used as an auxiliary parameter along with the capillary forces to assemble particles at fluid interfaces or in the bulk. Finally, we present examples how these interactions can be used jointly in magnetically responsive foams, gels, and pastes for 3D printing. The multiphasic particle gels for 3D printing open new opportunities for making of magnetically reconfigurable and “active” structures. 

It is challenging to find a conventional nanofabrication technique that can consistently produce soft polymeric matter of high surface area and nanoscale morphology in a way that is scalable, versatile, and easily tunable. Here, the capabilities of a universal method for fabricating diverse nano‐ and micro‐scale morphologies based on polymer precipitation templated by the fluid streamlines in multiphasic flow are explored. It is shown that while the procedure is operationally simple, various combinations of its intertwined mechanisms can controllably and reproducibly lead to the formation of an extraordinary wide range of colloidal morphologies. By systematically investigating the process conditions, 12 distinct classes of polymer micro‐ and nano‐structures including particles, rods, ribbons, nanosheets, and soft dendritic colloids (dendricolloids) are identified. The outcomes are interpreted by delineating the physical processes into three stages: hydrodynamic shear, capillary and mechanical breakup, and polymer precipitation rate. The insights into the underlying fundamental mechanisms provide guidance toward developing a versatile and scalable nanofabrication platform. It is verified that the liquid shear‐based technique is versatile and works well with many chemically diverse polymers and biopolymers, showing potential as a universal tool for simple and scalable nanofabrication of many morphologically distinct soft matter classes.

 

The design of hydrogels where multiple interpenetrating networks enable enhanced mechanical properties can broaden their field of application in biomedical materials, 3D printing, and soft robotics. We report a class of self-reinforced homocomposite hydrogels (HHGs) comprised of interpenetrating networks of multiscale hierarchy. A molecular alginate gel is reinforced by a colloidal network of hierarchically branched alginate soft dendritic colloids (SDCs). The reinforcement of the molecular gel with the nanofibrillar SDC network of the same biopolymer results in a remarkable increase of the HHG’s mechanical properties. The viscoelastic HHGs show >3× larger storage modulus and >4× larger Young’s modulus than either constitutive network at the same concentration. Such synergistically enforced colloidal-molecular HHGs open up numerous opportunities for formulation of biocompatible gels with robust structure-property relationships. Balance of the ratio of their precursors facilitates precise control of the yield stress and rate of self-reinforcement, enabling efficient extrusion 3D printing of HHGs.