Nanocomposites with ordered bridged solid-liquid structures are prepared through a dual-material direct ink writing technique, using high-viscosity silicone rubber as the solid-phase ink and carbon black/low-viscosity silicone rubber as the liquid-phase ink. The printability of the two inks is evaluated by rotational rheometer, and the structures of the composites are characterized by optical microscopy and micro-CT. Tensile properties, electrical conductivity, and electromagnetic interference (EMI) shielding effectiveness of the composites are investigated. The results show that the elongation at break, conductivity, and EMI shielding effectiveness increase with the increased bridging span of the liquid bridge, exhibiting high values up to 233%, 0.45 S/m, and 25 dB, respectively. Besides, negligible performance degradation is observed for the nanocomposites at external deformations, because the conductive liquid bridge remains always connected, giving it a great potential in applications such as flexible EMI shielding devices.