The development of biomass-based composites has greatly reduced the daily consumption of plastics. However, these materials are rarely recyclable, thus, posing a severe threat to the environment. Herein, we designed and prepared novel composite materials with ultra-high biomass (i.e., wood flour) filling capacity and good closed-loop recycling properties. The dynamic polyurethane polymer was polymerized in situ on the surface of wood fiber, and then they were hot-pressed into composites. Fourier-transform infrared (FTIR), scanning electron microscopy (SEM), and dynamic thermomechanical analysis (DMA) measurements reveal good compatibility between the polyurethane and wood flour in the composites when the wood flour content is ≤80 wt%. The maximum tensile and bending strength of the composite are 37 and 33 MPa when the wood flour content is 80%. The higher wood flour content results in higher thermal expansion stability and creep resistance in the composites. Moreover, the thermal debonding of dynamic phenol–carbamate bonds facilitates the composites to undergo physical and chemical cycling. The recycled and remolded composites exhibit good mechanical property recovery rates and retain the chemical structures of the original composites.

In this study, alkali-treated wood flour/dynamic polyurethane composites were successfully prepared through a solvent-free one-pot method and in situ polymerization. The effects of the alkaline treatment process, changes in the flexible long-chain content in the dynamic polyurethane system, and the wood flour filling amount on the interface’s bonding, mechanical, and reprocessing properties were investigated. Partial removal of lignin and hemicellulose from the alkali-treated wood flour enhanced rigidity and improved interface bonding and mechanical strength when combined with dynamic polyurethane. The tensile strength was improved from 5.65–11.00 MPa to 13.08–23.53 MPa. As the composite matrix, dynamic polyurethane could not easily infiltrate all wood flour particles when its content was low or its fluidity was poor. Conversely, excessive content or overly high fluidity led to leakage and the formation of large pores, affecting the mechanical strength. As the polyol content increased, the matrix exhibited greater fluidity, which enabled it to accommodate more wood flour and penetrate the cell cavity or even the cell wall. This improved infiltration enhanced the interface bonding performance of the composites and made their mechanical properties sensitive to changes in wood flour content. The reprocessing ability of the prepared composites decreased with the increase in wood flour content, and the interface bonding was enhanced after reprocessing. The tensile strength retention rate of the composites prepared with alkali-treated wood flour was lower. This study provides a theoretical basis for optimizing the performance of wood fiber/dynamic polyurethane composites and an exploration path for developing self-healing and recyclable wood–plastic composites, which can be applied to building materials, automotive interiors, furniture manufacturing, and other fields.