The superconducting critical temperature (Tc > 15K) of niobium titanium nitride (NbTiN) thin films allows for low-loss circuits up to 1.1 THz, enabling on-chip spectroscopy and multi-pixel imaging with advanced detectors. The drive for large scale detector microchips is demanding NbTiN films with uniform properties over an increasingly larger area. This article provides an experimental comparison between two reactive d.c. sputter systems with different target sizes: a small target (100mm diameter) and a large target (127 mm x 444.5 mm). This article focuses on maximizing the Tc of the films and the accompanying I-V characteristics of the sputter plasma, and we find that both systems are capable of depositing films with Tc > 15 K. The resulting film uniformity is presented in a second manuscript in this volume. We find that these films are deposited within the transition from metallic to compound sputtering, at the point where target nitridation most strongly depends on nitrogen flow. Key in the deposition optimization is to increase the systems pumping speed and gas flows to counteract the hysteretic effects induced by the target size. Using the I-V characteristics as a guide proves to be an effective way to optimize a reactive sputter system, for it can show whether the optimal deposition regime is hysteresis-free and accessible.