A low-temperature (>450 °C) thermal chemical vapor deposition (CVD) process was developed for the growth of TaNx from the reaction of tantalum pentabromide, ammonia, and hydrogen. Studies of process reaction kinetics yielded two sequential rate-controlling steps, with an activation energy of 0.45 eV for the kinetically limited reaction regime. Additionally, a systematic design of experiments approach examined the effects of key process parameters, namely, substrate temperature, source temperature, and hydrogen and ammonia flows, on film properties. A wide CVD process window was established for nitrogen-rich amorphous TaNx with contamination below 1 at.%. Film conformality was higher than 95% in nominally 0.30 μm, 4.5: 1 aspect ratio, trench structures.