Recently, some attempts have been made to enhance the gas barrier properties of semicrystalline polymers by precisely controlling the arrangement of their impermeable crystalline lamellae. However, it is still a great challenge to achieve regular arrangement of the lamellae along the direction perpendicular to the gas diffusion path, especially using conventional polymer processing technologies. This work presents a novel and simple strategy to dramatically improve oxygen barrier performance of biobased and biodegradable polylactide (PLA) through constructing parallel-aligned shish-kebab-like crystals with well-interlocked boundaries with the aid of a highly active nucleating agent. The nucleating agent was introduced into PLA by melting compounding and the sheet-like specimens were fabricated by compression molding. We demonstrate that the fibrillar nucleating agent dispersed in PLA melt can serve as shish to induce the change of crystallization habit of PLA from isotopic spherulitic crystals to unique shish-kebab-like crystals and the shear flow in the compression molding can induce the highly ordered alignment of the nucleating agent fibrils as well as the subsequent shish-kebab-like crystals along the direction parallel to the sheet surface. More importantly, the growing lamellae are found to interpenetrate and tightly interlock with each other at the boundary regions of the shish-kebab-like crystals in the later stage of the crystallization, forming a densely packed nanobrick wall structure to prevent gas molecules from permeating through the crystals and thus imparting the PLA sheets with unprecedentedly low oxygen permeability. This work provides not only a successful example of preparing semicrystalline polymer with super gas barrier properties by tailoring crystal superstructure but also a promising route to rapidly fabricate high-performance food packaging materials via industrially meaningful melt processing.