MX monopnictide compounds (M=Nb,Ta, X = As,P) are prototypical three-dimensional Weyl semimetals (WSMs) that have been shown in bulk single crystal form to have potential for a wide variety of novel devices due to topologically protected band structures and high mobilities. However, very little is known about thin film synthesis, which is essential to enable device applications.We synthesize TaAs(001) epilayers by molecular beam epitaxy on GaAs(001) and provide an experimental phase diagram illustrating conditions for single phase, single-crystal-like growth. We investigate the relationship between nanoscale defects and electronic structure, using angle-resolved photoemission spectroscopy, Kelvin probe microscopy and transmission electron microscopy. Our results provide a roadmap and platform for developing 3D WSMs for device applications.