This study provides an overview of the atmospheric drivers of climate change over Greece (Eastern Mediterranean), focusing on greenhouse gases (GHG: carbon dioxide, CO2; methane, CH4; etc.). CO2 in Greece is mostly produced by energy production, followed by transport, construction, and industry. Waste management is the largest anthropogenic source of methane, accounting for 47% of total CH4 emissions, surpassing emissions from the agricultural sector in 2017, while the energy sector accounts for the remaining 10.5%. In situ simultaneous observations of GHG concentrations in Greece conducted at three sites with different topologies (urban background; Athens, regional background; Finokalia and free troposphere; and Helmos) during the last 5 years (2019–2023) showed increasing trends of the order of 2.2 ppm·yr−1 and ~15 ppb·yr−1 for CO2 and CH4, respectively, in line with the global trends. These increasing trends were found from both ground-based and satellite-based remote-sensing observations. Finally, during the lockdown period due to the COVID-19 global pandemic, a 58% reduction in CO2 levels was observed in the urban background site of Athens after subtracting the regional background levels from Finokalia, while the respective reduction in CH4 was of only the order of 15%, highlighting differences in emission sources.