The region of Al-Jabal Al-Akhdar in northeastern Libya has undergone rapid, wide-ranging changes in the land use and land cover (LULC) intensified by the conversion of natural resources for food purpose, urbanization, and other socioeconomic benefits. This study examined the use of geographic information system (GIS) and remote sensing techniques to gain a quantitative understanding of the spatiotemporal dynamics of LULC. In addition, the major factors behind LULC changes and decline of natural vegetation in the region were analyzed. A post-classification comparison approach was used to detect LULC changes in the study area between 1985 and 2017 using four Landsat images from 1985, 2000, 2010, and 2017. The observed changes were indicative of a decrease in the expanse of the natural Mediterranean forest which lost 9018 ha over 32 years, 39% of its total area, with the highest deforestation rate registered between 2010 and 2017 estimated at 513 ha. year−1. Orchards and rain-fed agriculture lands gained 4095 ha, which matches 55% of initial area, whereas the land under irrigated crops increased by 2266 ha, about 85% of the original area. The area of urban and built-up land in 2017 was more than double in 1985 and achieved the highest urbanization rate between 2010 and 2017 at 203 ha.year−1. Results indicate an unstable trend of bare and low vegetation lands which generally increased by about 50%. From the outcomes of this research, it is strongly recommended that urgent measures be taken to conserve the natural forest and to achieve a rational use of agricultural land in the region of Al-Jabal Al-Akhdar.