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Sr2+-doped cerium pyrophosphate (Ce1–x Sr x P2O7, x = 0.05, 0.1, 0.15, and 0.2) electrolytes are synthesized by digesting cerium oxide and strontium nitrate with 85% H3PO4. The ionic conductivity behavior of Ce1–x Sr x P2O7-sintered pellets is analyzed by electrochemical impedance spectroscopy in a dry and humid air atmosphere. The time-dependent variation of ionic conductivity during humidification process and the variation of conductivity with temperature are studied. In humid atmosphere in the 90–230 °C range, the variation of ionic conductivity is explained on the basis of the combined effect of ionic mobility and the availability of charge carriers in the samples. The ionic conductivity shows dependence on dopant concentration and water vapor pressure (pH2O). In dry air, conductivity of Ce1–x Sr x P2O7 is very low, with Ce0.9Sr0.1P2O7 showing a maximum conductivity of 4.3 × 10–6 S/cm at 430 °C. Among various Ce1–x Sr x P2O7 samples, Ce0.9Sr0.1P2O7 shows the highest conductivity in humid air (pH2O = 0.12 atm) with a maximum conductivity of 6.3 × 10–3 S/cm at 90 °C, and the conductivity of Ce0.9Sr0.1P2O7 was 3.5 × 10–3 S/cm at 190 °C and pH2O = 0.12 atm. On the basis of XRD results, the stability of Ce1–x Sr x P2O7 in a humid atmosphere is analyzed.