Electrohydrodynamic (EHD) pattern formation in carbon nanotube-polymer composite films yields well-defined patterns on the micrometer scale along with the alignment of carbon nanotubes (CNTs) within these patterns. Conductive pathways in nanotube networks formed during EHD patterning of nanocomposite films results in a substantial increase in the composites’ conductivity at loadings exceeding the percolation threshold. The degree of nanotube alignment can be tuned by adjusting the EHD parameters and the degree of alignment is mirrored by the conductivity across the film. Using etching techniques or by embedding relatively long nanotubes, patterned surfaces decorated by CNT brushes were generated.