Piezoelectric materials are currently among the most promising building blocks for sensing, actuation and energy harvesting systems. However, these materials are limited in certain applications due to their lack of machinability as well as their inability to conform to curved surfaces. One method to mitigate this issue is through additive manufacturing (direct printing) of piezoelectric nanocomposites, where piezoelectric nanomaterials are embedded in a polymer matrix. Although significant progress has been made in this area, filler morphology, alignment and volume fraction are critical parameters that influence the electromechanical response and have not been adequately modeled. With the advent of additive manufacturing it is now possible to realize directly printed nanocomposites with tailored microstructure. The objective of this study is to develop and experimentally validate micromechanical and finite element models that allow the study of the electroelastic properties of a directly printed nanocomposite containing piezoelectric inclusions. Furthermore, the dependence of these properties on geometrical parameters such as aspect ratio and alignment of the active phase are investigated. In particular, the core focus of this work is to demonstrate how the gradual alignment of piezoelectric nanowires in the nanocomposite from randomly oriented to purely aligned can improve electroelastic properties of a printed nanocomposite. Finally, this work provides the first experimental validation of the theoretical and FEM models through measurement of the electroelastic properties of the nanocomposites containing barium titanate nanowires in a polydimethylsiloxane (PDMS) polymer matrix.