Ice‐Templating of Core/Shell Microgel Fibers through ‘Bricks‐and‐Mortar’ Assembly**

A ‘bricks-and-mortar’ assembly approach can be used to create well- defined fibers on the microscale with alternating organic-inorganic arrangement through a simple ice-templating strategy. The fibers are constructed from closely packed monodisperse inorganic nanoparticles@PNIPAm core/shell microgels. A series of functional ‘bricks’, such as core/shell and hollow nanoparticles are prepared.