This paper presents a comparative study on the burst pressure performance of aluminum (Al) liner for Type-III composite overwrapped pressure vessels (COPVs). In the analysis, the vessels were loaded with increasing internal pressure up to the burst pressure level. In the analytical part of the study, the burst pressure of the cylindrical part was predicted based on the modified von-Mises, Tresca, and Average Shear Stress criterion (ASSC). In the numerical analysis, a finite element (FE) model was established in order to predict the behavior of the vessel as a function of increasing internal pressure and determine the final burst. The Al pressure vessels made of Al-6061-T6 alloy with a capacity of 5L were designed. The experimental study was conducted by pressurizing the Al vessels until the burst failure occurred. The results obtained through analytical, numerical and experimental work were compared. The average experimental burst pressure of the vessels was found to be 279 bar. The experimental strain data were compared with the results of the FE analysis. The results indicated that the FE analysis and ASSC-based elastoplastic analytical approaches yielded the best predictions which are within 2.2% of the experimental burst failure values. It was also found that the elastic analysis underestimated the burst failure results; however, it was effective for determining the critical regions over the vessel structure. The strain behavior of the vessels obtained through experimental investigations was well correlated with those predicted through FE analysis.