Herein, the Mn1.95-xCo0.21Ni0.84SrxO4 (MCNS) (0 ≤ x ≤ 0.15) based negative temperature coefficient (NTC) materials are prepared by co-precipitation method. The replacement of Mn by Sr plays a critical role in controlling the lattice parameter, relative density, microstructure and electrical properties. The lattice parameter and relative density increase with the increase of Sr content. A small amount of Sr restrains the grain growth and increases the bulk density. Moreover, the ρ25, B25/50, Ea and α values of MCNS ceramics are influenced by the Sr content and ranged from 1535.0-2053.6 Ω·cm, 3654-3709 K, 0.3149-0.3197 eV and -4.111--4.173%, respectively. The XPS results explain the transformation of MCNS ceramics from n- to p-type semiconductors. The conduction could arise from the hopping polaron between Mn3+/Mn4+ and Co2+/Co3+ in the octahedral sites. The impedance data analysis also discussed the conduction mechanism of the MCNS ceramic, while grain resistance dominates the whole resistance of the samples. Furthermore, the aging coefficient (△R/R) of MCNS ceramics is found to be < 0.2%, which indicates the stable distribution of cations in the spinel. Finally, the MCNS ceramics demonstrate excellent thermal durability with <1.3% of resistance shift after 100 thermal shock cycles.