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With the growing requirement for lightweight structural materials in automotive, aerospace, and infrastructure applications, multi‐material joints made with adhesive have attracted intense research interest. Commercial thermoset adhesives are one‐time cures, and difficult to disassemble the bonded components for repair and recycling. Our prior work with a thermoplastic acrylonitrile‐butadiene‐lignin rubber (ABL) addresses this sustainability/recycling challenge, but the adhesive exhibits deficient joining strength compared to standard thermosets. Here, we modify the ABL matrix by loading particulate fillers to enhance its modulus and toughness. The goal is to manufacture a cure‐free thermoplastic adhesive system with a simple dispensing protocol and characteristic ductility combined with a high yield stress for improved shear strength of a bonded joint. Fumed silica (FS) and epoxidized glass spheres (EGS) were used as fillers in the ABL to promote the dispersion of lignin particles that tailored the functionalities and free energy components of the adhesive surface. With optimal loading of FS (5 wt%) and EGS (30 wt%) in the ABL adhesive matrix, the lap‐shear strength of the bonded aluminum joint was elevated by 128%, compared to the neat ABL, reaching 21 MPa, which is 90% of the performance of a commercial epoxy‐based adhesive. Highlights: A partly renewable filler‐toughened thermoplastic adhesive has been developed.This thermoplastic gives nearly equivalent performance of adhesively bonded aluminum joint compared to standard thermosets.Experimental and simulation data help understand the adhesive reinforcing mechanism by the fillers. [ABSTRACT FROM AUTHOR]

The cover image is based on the Research Article Acrylonitrile‐butadiene‐lignin thermoplastic rubber adhesive for enhanced metal‐to‐metal joining by Zeyang Yu et al., https://doi.org/10.1002/pc.28258. [ABSTRACT FROM AUTHOR]