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The demand for biopolymer-based green packaging has attracted growing attention because of its outstanding properties and consistency with clean environmental principle, unfortunately, its slow crystallization rate and narrow processing window are challenging. Inspired by combined functions in nanocellulose-based conductive hybrids, this work developed high-performance polylactic acid (PLA) composites using conductive cellulose nanofiber (CNFene). Interestingly, CNFene has multiple functions as highly graphitized carbon and abundant hydroxyl groups, delivering stimulating properties to PLA composites. As nucleating agents, 3 wt% CNFene has a carbon layer on the surface combined with a hydrogen bonding network synergistically enhancing the tensile and crystallization properties of PLA-C3, with a tensile strength of ∼ 53.7 MPa, crystallinity of ∼ 33.9 %, and 6.6 °C decrease in the cold crystallization temperature. Additionally, the compatibility between CNFene and PLA can form a multi-level "reinforcement" network structure, further improving thermal stability and barrier properties. The resultant PLA-C3 showed higher thermal decomposition onset temperature (T 0), wider melt-processing window (197.6 °C) and extremely lower overall migration levels in ethanol (68.6 μg/kg) and isooctane (16.3 μg/kg), due to that improved interaction between CNFene and PLA positively affects crystallization ability and kinetic/mechanism of PLA to meet the requirements of industrial and green biopackaging applications. [Display omitted] [ABSTRACT FROM AUTHOR]