The influence of the coordination of (reversible) cross-links on the mechanical properties of aligned fiber bundles is investigated. Two polymeric systems containing cross-links of different coordination (two- and three-fold coordination) but having the same binding energy are investigated. In particular, the response to loading of these systems is compared. Mechanical parameters (strength, stiffness and work-to-fracture) are obtained by computational loading tests. The influence of coordination is studied for simple test systems with pre-defined topologies that maximize strength as well as for more realistic fiber bundles containing nine chains. The results show that a higher coordination of cross-links has a beneficial effect on the strength and the stiffness of the systems, while the work-to-fracture was found larger for the system having a smaller coordination of cross-links. It can be concluded that controlling the coordination of cross-links is a versatile tool to specifically tailor the mechanical properties of polymeric structures.