An aerosol jet printing (AJP) printing head built on top of precise motion systems can provide positioning deviation down to 3 μm, printing areas as large as 20 cm × 20 cm × 30 cm, and five-axis freedom of movement. Typical uses of AJP are 2D printing on complex or flexible substrates, primarily for applications in printed electronics. Nearly all commercially available AJP inks for 2D printing are designed and optimized to reach desired electronic properties. In this work, we explore AJP for the 3D printing of free-standing pillar arrays. We utilize aryl epoxy photopolymer as ink coupled with a cross-linking “on the fly” technique. Pillar structures 550 μm in height and with a diameter of 50 μm were 3D printed. Pillar structures were characterized via scanning electron microscopy, where the morphology, number of printed layers and side effects of the AJP technique were investigated. Satellite droplets and over-spray seem to be unavoidable for structures smaller than 70 μm. Nevertheless, reactive ion etching (RIE) as a post-processing step can mitigate AJP side effects. AJP-RIE together with photopolymer-based ink can be promising for the 3D printing of microstructures, offering fast and maskless manufacturing without wet chemistry development and heat treatment post-processing.