Mono‐Materials Created by Engineering a Continuum of P3HB Stereomicrostructures in a One‐Step Catalytic Process

Multi‐material products that combine multiple complementary polymers can create products with desired performance but present challenges to end‐of‐life (EoL) management. The emerging mono‐material product design based on a single polymer type addresses the fundamental EoL issue, but challenges of delivering vastly tunable material properties by the single polymer still remain. Here, we introduce a simple strategy to produce biodegradable poly(3‐hydroxybutyrate) (P3HB) materials with a wide range of material properties by engineering a stereomicrostructure continuum, achieved through polymerizing diastereomeric mixtures of racemic and meso ‐dimethyl diolides at various feed ratios with a single catalyst. This one‐step, one‐pot process produces biodegradable P3HB mono‐materials ranging from rigid to flexible thermoplastics, to tough thermoplastic elastomers, to a pressure‐sensitive adhesive (PSA), which have been then combined to fabricate prototype all‐P3HB PSA tapes, demonstrating the feasibility of designing mono‐material products through engineering polymer stereomicrostructures.