The rheological behavior and printing characteristics of the screen-printing slurry for Nd-Fe-B grain boundary diffusion are key factors that determine the quality of printing and magnetic performance. However, few studies have focused on the organic medium, a crucial material for slurry. In this paper, the rheology, thixotropy, and thermal decomposition behavior of the organic vehicle in Nd-Fe-B screen printing slurry were studied. The results show that the organic vehicle formed by terpineol and polyvinyl butyral (PVB) exhibits typical non-Newtonian fluid characteristics, with excellent rheology and thixotropy, ensuring that the slurry prepared from it has excellent static stability and printing consistency. Additionally, the carbon residue of the organic vehicle formed by terpineol and PVB is less than 0.1% at 900 °C, avoiding excessive carbon entering the magnet during the diffusion process. Moreover, studying the rheology and thixotropy of the organic vehicle through a rheometer can quickly screen the slurry system. This work provides valuable guidance for designing an organic vehicle for screen-printing slurry for Nd-Fe-B grain boundary diffusion in future research.