Carbon nanotubes (CNTs) embedded in carbon/epoxy (c/ep) composites offer a lightweight, stiff solution with high damping for structural components. To manufacture CNT/c/ep hybrid composites with high concentrations of CNTs, a CNT yarn interlayer concept is used. Through a mechanism known as stick-slip, the interface between CNTs and c/ep laminates dissipate energy during dynamic cycling. It is predicted that altering the interfacial bond strength can enhance dynamic properties: loss factor, loss modulus, and storage modulus. In this research, the effect of surface treatments on CNT yarns prior to inserting the CNTs into the laminate was explored to determine if the dynamic properties of the composite were enhanced. It was determined that 2,3-dibromo-1,4-butanediol (23D14B), Triton X-100 (TX) and a solution of sulfuric and nitric (S/N Acid) were the best treatments of 12 tested based on the increased dynamic properties. For a composite with 5 vol% CNT yarn interlayers, 23D14B, TX, and S/N Acid increased Loss Factor by 230%, 130%, and 160%, respectively. Elevated temperature, moisture-saturated/elevated temperature, and cyclic loading frequency were investigated on 5vol. % CNT interlayers to determine their effects on dynamic properties of the CNT hybrid composites.