This paper investigates the optimal observational array for improving the prediction of the El Niño-Southern Oscillation (ENSO) by exploring sensitive areas for target observations of two types of El Niño events in the whole Pacific. A target observation method based on the particle filter and pre-industrial control runs from six coupled model outputs in Coupled Model Intercomparison Project Phase 5 (CMIP5) experiments are used to quantify the relative importance of the initial accuracy of sea surface temperature (SST) in different Pacific areas. The initial accuracy of the tropical Pacific, subtropical Pacific, and extratropical Pacific can all exert influences on both types of El Niño predictions. The relative importance of different areas changes along with different lead times of predictions. Tropical Pacific observations are crucial in decreasing the root mean square error of predictions of all lead times. Subtropical and extratropical observations play an important role in decreasing the prediction uncertainty, especially when the prediction is made before and throughout boreal spring. To consider different El Niño types and different start months for predictions, a quantitative frequency method based on frequency distribution is applied to determine the optimal observations of ENSO predictions. The final optimal observational array contains 31 grid points, including 21 grid points in the equatorial Pacific and 10 grid points in the north Pacific, suggesting the importance of the initial SST conditions for ENSO predictions not only in the tropical Pacific but also in the area outside the tropics. Furthermore, the predictions made by assimilating SST in sensitive areas have better prediction skills in the verification experiment, which can indicate the validity of the optimal observational array designed in this study.