In this paper, bulk polymeric composites with staggered orientation of carbon nanotubes (CNTs) in polymer matrix were prepared by means of a macro layer-by-layer (MLBL) method, while an alternating current (AC) electric field was applied for inducing alignment of the CNTs. Test results verified that there existed a relationship between conductive capacity of the composites and orientation of the CNTs in matrix. Conductivity of the composites containing aligned CNTs represented a dependency on time and testing history on the composite specimens. Among the composites with different orientation types of CNTs in the matrices, the composite specimens including staggered orientation of CNTs in polymer matrix demonstrated the most outstanding electric conductivity and showed similar conductive properties in the two directions of the CNT alignment.