Drop-on-demand inkjet printing of functional inks has received a great deal of attention for realizing printed electronics, rapidly prototyped structures, and large-area systems. Although this method of printing promises high processing speeds and minimal substrate contamination, the performance of this process is often limited by the rheological parameters of the ink itself. Effective ink design must address a myriad of issues, including suppression of the coffee-ring effect, proper drop pinning on the substrate, long-term ink reliability, and, most importantly, stable droplet formation, or jettability. In this work, by simultaneously considering optimal jetting conditions and ink rheology, we develop and experimentally validate a jettability window within the capillary number−Weber number space. Furthermore, we demonstrate the exploitation of this window to adjust nanoparticle-based ink rheology predictively to realize a jettable ink. Finally, we investigate the influence of mass loading on jettability to establish additional practical limitations on nanoparticle ink design.