Plant cells sequester atmospheric carbon in thick walls containing heterogenous networks of cellulose and hemicelluloses (e.g. xylan and mannan), surrounded by additional polymers. Plants and microbes secrete glycosyl hydrolases that act alone or as modular complexes to modify extracellular polysaccharides. While several carbohydrate-active enzymes have been successfully targeted for crop improvement, additional hydrolytic proteins or more efficient versions are needed for the circular bioeconomy. Here, we discuss persistent challenges and emerging opportunities to enhance extracellular enzymes for use in plants or as tools to process biomass for various products. In addition to the design of minimal cellulosomes that combine microbial scaffolding proteins and polysaccharide-degrading enzymes, we review three major strategies that could improve the properties of plant-derived glycosyl hydrolases.
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