Bio‐inspired Heterostructured Bead‐on‐String Fibers That Respond to Environmental Wetting

Inspired by the geometric structure of ecribellate spider capture silk and its spinning characteristics, we propose a one‐step electrohydrodynamic method to fabricate bead‐on‐string heterostructured fibers (BSHFs). By combining electrospinning and electrospraying strategies using a sprayable outer fluid with low viscosity and a spinnable inner fluid with high viscosity in a coaxial jetting process, hydrophilic poly(ethylene glycol) beads are successfully imprinted on a hydrophobic polystyrene string. It is demonstrated that the BSHFs are capable of intelligently responding to environmental change. With a change in relative humidity, the fibers show a segmented swelling and shrinking behavior in the “bead” parts whereas the “string” parts remain the same. The elastic BSHFs with alternating hydrophilic and hydrophobic surface characteristics represent a type of mesoscale analogues that block copolymers and may bring about new properties and applications. Moreover, the combined electrohydrodynamic approach developed herein should open new routes to multifunctional one‐dimensional heterostructured materials.