In this paper, a new approach for characterizing dispersion in nano-enhanced polymers and polymer composites using nanomechanical characterization is developed. Dispersion of Carbon nanofibers (CNFs) as a model nanoscale ingredient is characterized in two model polymer systems: (a) a thermoplastic polymer processed using a Twin Screw Extruder, and (b) a thermoset epoxy processed using sonication during solvent processing. For the first time, the modulus of agglomerated nanofibers was isolated from the polymer matrix enhanced with dispersed nanofibers by using nanomechanical characterization. Thus, it was possible to use these nanomechanical properties in a microstructural model using a Rule-of-Mixtures (ROM) formulation to determine the fraction of dispersed nanofibers, which yielded a dispersion limit of 3 vol% CNFs in the nano-enhanced thermoplastic polymer and 3.5 vol% CNFs in the nano-enhanced thermoset epoxy. It was also possible to predict the modulus measured using microtensile testing, and to determine an effective modulus of 30 GPa for the CNFs, which was attributed to a spring-like effect from kinking along the nanofibers. Applying this characterization to control of dispersion through sonication in the nano-enhanced thermoset epoxy, it was possible to determine the degree of dispersion with sonication time which was described using an Avrami equation. Finally, a carbon-fiber mat was used to create a model nano-enhanced polymer composite whose properties were found to be insensitive to sonication time due to filtering effects from the carbon-fiber mat and varied with CNF concentration in a manner where the CNF modulus could be extrapolated to 30 GPa, consistent with the nano-enhanced polymers.