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Renewable and biodegradable materials derived from biomass are attractive candidates to replace non-biodegradable petrochemical plastics. However, the mechanical performance and wet stability of biomass are generally insufficient for practical applications. Herein, we report a facile in situ lignin regeneration strategy to synthesize a high-performance bioplastic from lignocellulosic resources (for example, wood). In this process, the porous matrix of natural wood is deconstructed to form a homogeneous cellulose-lignin slurry that features nanoscale entanglement and hydrogen bonding between the regenerated lignin and cellulose micro/nanofibrils. The resulting lignocellulosic bioplastic shows high mechanical strength, excellent water stability, ultraviolet-light resistance and improved thermal stability. Furthermore, the lignocellulosic bioplastic has a lower environmental impact as it can be easily recycled or safely biodegraded in the natural environment. This in situ lignin regeneration strategy involving only green and recyclable chemicals provides a promising route to producing strong, biodegradable and sustainable lignocellulosic bioplastic as a promising alternative to petrochemical plastics. There is growing interest in the development of biodegradable plastics from renewable resources. Here the authors report an in situ process involving only green chemicals to deconstruct natural wood, forming lignocellulosic bioplastics that are mechanically strong, stable against water and sustainable.