Carbon nanomaterials are consistently providing new excitement over their properties and potential applications, but many of these material have yet to fully live up to their expectations commercially. The barrier to adoption often exists as a result of complex processing, fragility of the as-produced material, or difficulty scaling beyond laboratory quantities. This work provides a new approach for utilizing fibrous carbon nanomaterials to advance the technology toward new applications and industrial utility. This is accomplished by creating tailored device architectures through in-situ integration of activated carbon powder using carbon nanofiber deposition. The resulting hybrid materials and components can serve in diverse applications, with each instance able to be fine-tuned through a combination of processing parameters. The applications of such materials are anticipated to directly serve current carbon-based technology in filtration, energy storage and delivery, and thermal management, but the concepts are not limited to current carbon applications.