The Global Human Settlement Population Grid (GHS-POP) the latest released global gridded population dataset based on remotely sensed data and developed by the EU Joint Research Centre, depicts the distribution and density of the total population as the number of people per grid cell. This study aims to assess the GHS-POP data accuracy based on root mean square error (RMSE), mean absolute error (MAE), and mean absolute percentage error (MAPE) and the correlation coefficient. The study was conducted for Poland and Portugal, countries characterized by different population distribution as well as two spatial resolutions of 250 m and 1 km on the GHS-POP. The main findings show that as the size of administrative zones decreases (from NUTS (Nomenclature of Territorial Units for Statistics) to LAU (local administrative unit)) and the size of the GHS-POP increases, the difference between the population counts reported by the European Statistical Office and estimated by the GHS-POP algorithm becomes larger. At the national level, MAPE ranges from 1.8% to 4.5% for the 250 m and 1 km resolutions of GHS-POP data in Portugal and 1.5% to 1.6%, respectively in Poland. At the local level, however, the error rates range from 4.5% to 5.8% in Poland, for 250 m and 1 km, and 5.7% to 11.6% in Portugal, respectively. Moreover, the results show that for densely populated regions the GHS-POP underestimates the population number, while for thinly populated regions it overestimates. The conclusions of this study are expected to serve as a quality reference for potential users and producers of population density datasets.