Remote sensing has been shown to be a useful tool in retrieval aerosol optical thickness (AOT) in particulate matter (PM) pollution monitoring. In this study, daily AOT data retrieved from moderate resolution IMAGING spectroradiometer (MODIS) and the amount of PM10 measured at eight air quality monitoring ground stations in Klang Valley from 2004 to 2006 were used. The AOT values consisted of three different average window sizes (WS): (3 × 3) pixels, (5 5) pixels and (7 × 7) pixels. PM10 mass concentration consists of real-time (hourly) and 24 h mean. Linear correlation coefficients (LCC) were used to determine the best validation result. Best validation results were obtained between AOT WS in (5 × 5) pixels and PM10 mass in 24 h mean. The LCCs in dry season were acquired higher than those in rainy season. The validation results in rainy season were improved when nonlinear correlation coefficients (NLCC) with polynomial equation were used for analysis. This study reveals that the correlation coefficients are dependent on time and location.