This study investigates the effects of post-curing temperatures on the tensile properties of hybrid basalt-jute-glass-carbon fiber-reinforced polymers (FRPs). Composite specimens were post-cured at 60 °C and 100 °C for 60 min, and their tensile behavior was assessed using a servo-hydraulic testing machine. Numerical simulations using the Abaqus software V6.14 were also conducted to compare experimental and computational results. The findings indicate that post-curing heat treatment enhances ductility due to increased polymer cross-linking, but excessive heat treatment at 100 °C negatively impacts elongation at fracture. The results revealed that specimens post-cured at 60 °C exhibited the optimal balance between strength and ductility, with increased elongation and moderate tensile strength. However, at 100 °C, while tensile strength improved in some cases, a significant decrease in elasticity and an increased risk of brittleness were observed, suggesting that extreme heat treatment may degrade polymer integrity. Natural fiber composites, particularly jute-based samples, outperformed synthetic composites in terms of elongation and overall mechanical stability. The numerical simulations provided further insights but showed discrepancies with experimental results, mainly due to fiber property variations and fabric waviness, underscoring the challenges of accurately modeling woven composites. The study highlights the importance of controlled post-curing temperatures in optimizing the mechanical performance of FRP composites, with 60 °C identified as the most effective condition for achieving a favorable balance between tensile strength, flexibility, and material durability. These findings offer valuable insights for material scientists and engineers working on the development of high-performance composite materials for structural and industrial applications.