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[Display omitted] • The ternary composites containing PLLA, PBAT and CNFs were prepared. • PBAT and CNFs assembled into the "mutton kebab"-like structure during processing. • CNFs induced the epitaxial crystallization of PLLA on the surface of CNFs. • Highly-toughened, high heat resistant and self-healing properties were achieved. Biodegradable poly(L -lactic acid) (PLLA) based blend composites with excellent toughness exhibit comprehensive applications and they can be substitute for the common polyolefin and polyester based composites. To date, various strategies have been developed to enhance the toughness of the PLLA based blends or composites. Here, carbon nanofibers (CNFs) incorporated PLLA/poly(butylene adipate-co-butylene terephthalate) (PBAT) blend composites were investigated. The crystallinity of the PLLA matrix were precisely tailored through annealing treatment. Interestingly, CNFs and PBAT particles self-assembled into the "mutton kebab"-like structure during processing. In addition, the annealing treatment facilitated the epitaxial crystallization of PLLA on the surface of CNFs that were not covered by PBAT due to the excellent heterogeneous nucleation effect of CNFs. Consequently, with the addition of 1 wt% CNFs and tailoring the blend composite with the PLLA crystallinity of about 32.6%, the impact strength of the composite was increased by 270% from 10.0 kJ/m2 to 37.0 kJ/m2. The toughening mechanisms were mainly connected with the greatly strengthened interfacial interaction between PLLA matrix and PBAT particles by CNFs through CNFs bridging effect and CNFs inducing PLLA crystallization, facilitating the transfer of stress under the load condition, especially at high PLLA crystallinity. Furthermore, it was found that CNFs exhibited outstanding photothermal conversion effect, which could endow the blend composites with mechanical-damage-healing ability. This work not only reveals the role of crystalline structure in toughening of the PLLA-based blend composites but also paves an effective way to prepare super-toughened, biodegradable, heat resistant and mechanical-damage-healing PLLA-based composites via tailoring the crystalline structure of the matrix. [ABSTRACT FROM AUTHOR]