As a “green” alternative for traditional petroleum-based polymers, bio-based and biodegradable poly(L-lactide) (PLLA) exhibits tremendous application potential in various fields because of its outstanding biocompatibility, excellent processability, and favorable mechanical strength. However, the large-scale adoption of PLLA as a commodity thermoplastic still faces some obstacles mainly associated with its poor heat resistance because the low crystallization rate makes it hard to crystallize during melt processing. In this contribution, we report a facile and robust strategy to address this obstacle via simultaneously tailoring crystal morphology and lamellae orientation with the aid of the nucleating agent (NA) that can be completely dissolved in PLLA melt and re-organize into fibrils upon cooling. These fibrils can act as nucleation templates to induce the crystallization of PLLA lamellae perpendicular to their long axis, thus inducing the formation of shish-kebab structure accompanied with the significantly accelerated crystallization. More importantly, by taking advantage of the preferred orientation of NA fibrils along the flow direction experienced in melt processing, highly orientated PLLA lamellae is formed in injection molding articles and melt spun fibers. In this way, significantly improved heat resistance and tensile strength are achieved. This work provides a good example of preparing high-performance PLLA products by using a fibrous nucleating agent as a template to tailor the crystal morphology and lamellae orientation.