Deep-sea structures will collapse/implode under hydrostatic pressure when the structure dives below a threshold, leading to structural instability and catastrophic failure. To better understand how the layup angle of composite cylindrical shells influences this instability threshold, the present work explores how composite cylinders can achieve the highest (optimum) critical collapse pressure under hydrostatic loading conditions. To perform this analysis, a closed-form analytical cylinder buckling solution developed by previous work is used in conjunction with different cylindrical geometrical configurations and composite properties for glass, carbon, and intraply-hybrid composite properties for woven and unidirectional structures. The results show that a composite structure's optimum layup configuration is unique to the structure's geometry and material system. However, general trends are observed for these different systems, such as how symmetric and asymmetric constructions place the axial-resistant layers near the neutral plane of the composite system. In addition, both constructions need an increase in shear-resistance layers as the L/D ratio decreases regardless of the material system. Lastly, the analytical approach presented in this work can be used to accurately determine the optimum layup angle for composite cylindrical structures that are subjected to external hydrostatic pressure.