Widespread adoption of carbon nanomaterials has been hindered by inefficient production and utilization. A recently developed method has shown possibility to directly synthesize bulk nanostructured nonwoven materials from catalytically deposited carbon nanofibers (CNFs). The basic manufacturing scheme involves constraining carbon nanofiber growth to create three-dimensionally featured, macroscale products. Although previously demonstrated as a proof of concept, the possibilities and pitfalls of the method at a larger scale have not yet been explored. In this work, the basic foundation for using the constrained formation of fibrous nanostructures (CoFFiN) process is established by testing feasibility in larger volumes (as much as 2000% greater than initial experiments) and by noting the macroscale carbon growth characteristics. It has been found that a variety of factors contribute to determining the basic qualities of the macroscale fiber collection (nonwoven material), and there are tunable parameters at the catalytic and constraint levels. The results of this work have established that monolithic structures of nonwoven carbon nanofibers can be created with centimeter dimensions in a variety of cross-sectional shapes. The only limit to scale noted is the tendency for nanofibers to entangle with one another during growth and self-restrict outward expansion to the mold walls. This may be addressed by pregrowing carbon before placement or selective placement of the catalyst in the mold.