We propose a pressure-induced flow (PIF) processing method for the simultaneous enhancement of strength, toughness, and heat resistance of biodegradable poly(butylene succinate) (PBS). The pressure and temperature were systematically adjusted to optimize the tensile strength of PBS. Under the optimized processing conditions, the structured PBS was characterized by relatively high strength of 89.5 MPa, toughness of 21.4 kJ·m−2, and improved heat resistance without deterioration of much of its ductility. Microscopic analyses witnessed denser and highly oriented crystalline domains along the flow direction caused by PIF processing. Detailed crystallization analysis made by 2D-WAXD and 2D-SAXS unraveled the extremely ordered PBS domains, which were featured by a significant increase in the orientation degree from 0.25 for the reference to 0.73 for PIF-processed PBS. Such a highly ordered microstructure substantially boosted the degree of crystallinity and heat-resistance temperature of PBS. We believe that our findings would offer a facile, green, and cost-effective approach for fabricating biodegradable polymers with outstanding properties and performance.