Natural
rubber (NR) material is indispensable in various fields
of our daily life, while its preparation usually involves toxic cross-linking
agents and energy-consuming vulcanization processes. The permanent
cross-linking network of NR products also makes its degradation and
recycling difficult. Herein, a fully biosourced, vulcanization-free
NR material is developed by simply introducing carrageenan (KC) in
the rubber matrix via a facile aqueous mixing method. The nonrubber
components (NRCs) on the rubber latex particles are of crucial importance
for this art as they can interact with KC by forming hydrogen bonding
between the functional groups of proteins in NRCs and the abundant
hydroxyl and sulfonate groups on KC molecules. As a result, KC is
selectively dispersed between the latex particles and forms a segregated
filler network. The special KC network and the good interfacial interaction
between KC and rubber promote strain-induced crystallization and endow
rubber composites with great mechanical properties. Moreover, the
obtained NR/KC composites exhibit an interesting thermal-responsive
attraction behavior, which has good potential in smart applications,
such as artificial muscle. This work paves a simple and effective
path to vulcanization-free NR by leveraging the inherent NRC on latex
rubber particles, opening a new horizon for the sustainable development
of NR/polysaccharide composite elastomers.