The alignment of high aspect ratio reinforcing nanoparticles within a polymer matrix can have significant effects on the mechanical, electrical, and thermal properties of the nanocomposite. Therefore, in order to tailor the properties of the composite, it is imperative to develop novel methods to control the alignment of these filler particles in various polymeric matrices. This paper reports a unique approach to alter the alignment of carbon nanotubes (CNT) within polydimethylsiloxane (PDMS) nanocomposites using 3D printing technology. A line of the reinforced PDMS resin is printed on a PDMS substrate using direct ink writing technology, which can produce alignment in the print direction depending on printing parameters, the loading of the reinforcing particle, and the rheology of the ink. Then, the substrate is stretched and placed in an oven to cure the printed nanocomposites line with increased alignment in the stretch direction. These two techniques have the advantage of simplicity over other techniques and can efficiently manufacture nanocomposites with the alignment of nanoparticles. Optical microscopy will be used to quantify the alignment within the printed line. Electrical and mechanical properties will be tested to determine the effects of the different alignments within the elastomer. The ability to control the alignment of elastomeric CNT composites is advantageous for the growing field of polymer-based electronics.