Development of biodegradable plastic materials is of primary importance in view of acute environmental and health problems associated with the accumulation of plastic waste. We fabricated a biodegradable composite material based on hydroxyethyl cellulose polymer and tyrosine nanocrystals, which demonstrates enhanced strength and ductility (typically mutually excluding properties), superior to most biodegradable plastics. This emergent behavior results from an assembly pattern that leads to a uniform nanoscale morphology and strong interactions between the components. Water-resistant biodegradable composites encapsulated with hydrophobic polycaprolactone as a protection layer were also fabricated. Self-assembly of robust sustainable plastics with emergent properties by using readily available building blocks provides a valuable toolbox for creating sustainable materials.