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A novel strategy adaptive to 3D printing of stereo-complexed polylactide matrix for simultaneous toughness and stiffness was designed. Stereo-complexation is a potent way to enhance both aqueous stability and heat resistance of polylactide, but also aggravates brittleness problem of polylactide. Though poly(butyleneadipate- co -terephthalate) elastomer with epoxidized compatibilizer improved stiffness and toughness of common polylactide, their effectiveness on mechanical and crystallization properties of stereo-complexed polylactide remained unknown. More importantly, incorporation of above techniques into 3D printing kept a fundamental challenge. Both stereo-complexation of polylactide and co valent coupling of polylactide and poly(butyleneadipate-co-terephthalate) by epoxidized compatibilizer are easy to occur when preparing the filaments for printing, impeding the following 3D printing procedure. The hypothesis for this research is that controlled hierarchical crystallization and reaction in three thermal processes could ensure simultaneous toughness and stiffness, and complete stereo-complexation in polylactide matrices. Reinforcing effects of a selected epoxidized compatibilizer, POSS (epoxy)8 , on crystallinities, thermal properties, mechanical properties and morphologies were systematically studied. Such a strategy not only removed the obstacles in incorporating stereo-complexation and coupling techniques of polylactide into 3D printing, but also revealed the mechanism to produce high-performance 3D printed polylactide matrix via hierarchical crystallization and reaction. • A novel strategy adaptive to 3D printing of stereo-complexed PLA was designed. • Hierarchical crystallization and reaction ensured feasibility of the strategy. • Improvement in composite ductility coincides with increase in strength. • Reinforcing effects of epoxidized POSS on PLA properties were systematically studied. • Complete stereo-complexation was achieved in 3D printed PLA matrices. [ABSTRACT FROM AUTHOR]