Multi-walled carbon nanotubes (MWCNTs)-reinforced polyurethane (PU) composites were fabricated by using solution mixing technique followed by compression molding. Nano dynamic mechanical analysis was carried out to investigate the viscoelastic properties of PU/MWCNTs composites within a frequency range of 5–250 Hz. At higher frequencies (250 Hz), the storage modulus of PU/MWCNTs composites with 10 wt% loading of MWCNTs was enhanced by 148% in equivalence to pristine PU. An improvement of 13.3% in storage modulus was observed at a loading frequency of 250 Hz in comparison to that of a loading frequency of 75 Hz, which indicates that the effect of MWCNTs on storage modulus was more pronounced at higher frequencies. At 75 Hz, a minor composition of MWCNTs (3 wt%) was sufficient to reduce the value of tan δ from 0.20 to 0.15, indicating that the material becomes more elastic after reinforcing MWCNTs. This significant improvement in the mechanical behavior of composite material has been attributed to the uniform dispersion of MWCNTs, and their adhesion with PU molecules. Reported enhancement in the elastic behavior of PU composite will boost the applicability of PU-based composite material for the fabrication of high-strength boots, gloves, and jackets required to absorb high vibration frequencies experienced during conditions such as rock drilling.