Concerns of petroleum dependence and environmental pollution prompt an urgent need for new sustainable approaches in developing polymeric products. Biobased polymers provide a potential solution, and biobased nanocomposites further enhance the performance and functionality of biobased polymers. Here we summarize the unique challenges and review recent progress in this field with an emphasis on self-assembly of inorganic nanoparticles. The conventional wisdom is to fully disperse nanoparticles in the polymer matrix to optimize the performance. However, self-assembly of the nanoparticles into clusters, networks, and layered structures provides an opportunity to address performance challenges and create new functionality in biobased polymers. We introduce basic assembly principles through both blending and in situ synthesis, and identify key technologies that benefit from the nanoparticle assembly in the polymer matrix. The fundamental forces and biobased polymer conformations are discussed in detail to correlate the nanoscale interactions and morphology with the macroscale properties. Different types of nanoparticles, their assembly structures and corresponding applications are surveyed. Through this review we hope to inspire the community to consider utilizing self-assembly to elevate functionality and performance of biobased materials. Development in this area sets the foundation for a new era of designing sustainable polymers in many applications including packaging, construction chemicals, adhesives, foams, coatings, personal care products, and advanced manufacturing.
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