Variously configured sub-laminate modules are provided, which comprise at least a first ply and a second ply, the first ply comprising fibers extending in a first orientation, the second ply comprising fibers extending in a second orientation. The second orientation is offset relative to the first orientation, which offset defines an acute angle between the two orientations. The acute angle is less than 90 degrees and in at least one embodiment, the acute angle is approximately 25°. In certain embodiments, the acute angle further defines an unbalanced structure of the sub-laminate module. In certain embodiments, the first and second plies may be further secured relative to one another in a non-crimped configuration. Composite laminated structures formed from various embodiments of the sub-laminate modules are also provided, at least some of which may be homogenized. Various methods of manufacturing the sub-laminate modules and the composite laminated structures are also provided.