Multiwalled, bamboo-like carbon nanotube (BCNT)/methyl vinyl silicone (MVQ) composites with different concentrations of BCNT were fabricated by liquid blending method with an aim to investigate the behavior of such composites as effective electromagnetic interference shielding material in the frequency range of 1-6GHz. The morphology and structure of BCNT were characterized and elucidated. Scanning electron microscopy examination showed that the BCNTs homogeneously dispersed in MVQ. The electrical conductivity (sigma) and shielding effectiveness (SE) of the composite were measured and discussed. The results showed that the BCNTs/MVQ composites had a relatively low percolation threshold at 0.92wt. % BCNT, and the sigma showed a decreasing linear relation with temperature, i.e., the sigma slightly decreased with increasing temperature. The BCNTs/MVQ composites with SE of 33-38dB were obtained at 7wt. % BCNT loading. Shielding mechanism was studied by resolving the total incident energy into absorbed, reflected, and transmitted contribution, and the result showed that the dominated shielding mechanism was reflection loss.