Urban Surface Ecological Status (USES) reflects the structure and function of an urban ecosystem. USES is influenced by the surface biophysical, biochemical, and biological properties. The assessment and modeling of USES is crucial for sustainability assessment in support of achieving sustainable development goals such as sustainable cities and communities. The objective of this study is to present a new analytical framework for assessing the USES. This analytical framework is centered on a new index, Remotely Sensed Urban Surface Ecological index (RSUSEI). In this study, RSUSEI is used to assess the USES of six selected cities in the U.S.A. To this end, Landsat 8 images, water vapor products, and the National Land Cover Database (NLCD) land cover and imperviousness datasets are downloaded for use. Firstly, Land Surface Temperature (LST), Wetness, Normalized Difference Vegetation Index (NDVI), and Normalized Difference Soil Index (NDSI) are derived by remote sensing methods. Then, RSUSEI is developed by the combination of NDVI, NDSI, Wetness, LST, and Impervious Surface Cover (ISC) with Principal Components Analysis (PCA). Next, the spatial variations of USES across the cities are evaluated and compared. Finally, the association degree of each parameter in the USES modeling is investigated. Results show that the spatial variability of LST, ISC, NDVI, NDSI, and Wetness is heterogeneous within and between cities. The mean (standard deviation) value of RSUSEI for Minneapolis, Dallas, Phoenix, Los Angeles, Chicago and Seattle yielded 0.58 (0.16), 0.54 (0.17), 0.47 (0.19), 0.63 (0.21), 0.50 (0.17), and 0.44 (0.19), respectively. For all the cities, PC1 included more than 93% of the surface information, which is contributed by greenness, moisture, dryness, heat, and imperviousness. The highest and lowest mean values of RSUSEI are found in “Developed, High intensity” (0.76) and “Developed, Open Space” (0.35) lands, respectively. The mean correlation coefficient between RSUSEI and LST, ISC, NDVI, NDSI, and Wetness, is 0.47, 0.97, −0.31, 0.17, and −0.27, respectively. The statistical significance of these correlations is confirmed at 95% confidence level. These results suggest that the association degree of ISC in USES modeling is the highest, despite the differences in land cover and biophysical characteristics in the cities. RSUSEI could be very useful in modeling and comparing USES across cities with different geographical, climatic, environmental, and biophysical conditions and can also be used for assessing urban sustainability over space and time.