In this research, we have studied the structural and electrical properties of NbTiN films deposited on MgO and SiO2/Si substrates by reactive dc sputtering. The formation of stoichiometric NbTiN is very sensitive to N concentration and can be easily adjusted by changing the discharge current and Ar: N2 ratio along the current–voltage curves (IVCs) of the NbTi target. Excessive or insufficient N concentration in NbTiN leads to sublattice expansion or distortion, resulting in a decrease in critical temperature T c. At Ar: N2 ratio of 30:4 and discharge current of 2.2 A, T c as high as 15.8 K and 15.3 K has been obtained for 200 nm thick NbTiN/MgO and NbTiN/SiO2/Si samples, respectively. In addition, the critical density J c of the 4 μm-wide and 7 nm-thick NbTiN film grown on MgO substrate at 2 K reaches 19.2 MA cm−2, which is approximately twice as high as the 10.9 MA cm−2 of the same-sized NbTiN film grown on SiO2/Si substrate. Therefore, by further fine-tuning the N concentration in combination with the IVCs of the target, high-quality stoichiometric NbTiN can be obtained.