Hybrid carbon fiber reinforced polymer composites are a new breed of materials currently being explored and characterized for next-generation aerospace applications. Through the introduction of secondary reinforcements, such as alumina nanoparticles, hybrid properties including improved mechanical properties—fracture toughness, for example—and stress-sensing capabilities can be achieved. However, problems with manufacturing can arise resulting from the inherent variability of the manufacturing techniques along with the tendency for the nanoparticles to agglomerate. Photoluminescence spectroscopy is used to investigate the effects of adjustments to manufacturing processes and silane functionalization on particle dispersion and sample consistency between samples of the same type. This work finds that application of surface treatments on the nanoparticles improved their dispersion, with the reactive treatment providing for the most consistency among samples. Improvements to dispersion and increased consistency resulting from specific changes in manufacturing processes were shown numerically. Findings provide a manufacturing recommendation to achieve optimum dispersion and mechanical properties of the composite.