Amid the dual objectives of “low carbon” and “ecological environmental protection”, focusing on Anhui Province, this study examined the spatial and temporal dynamics of land use carbon emissions (LUCE) and ecosystem service value (ESV) using grid analysis and models like GM and PLUS. The study highlights the substantial expansion of construction land from 2000 to 2020, witnessing a growth of 4726.92km2, primarily attributed to cultivated land, comprising 98.34% of the increase. Net carbon emissions exhibited an inverted “V”-shaped growth trend, surging by 10228.30×104 tons. The ESV in Anhui Province showed an “M”-shaped slow growth trend, with an increase of 1.14%. The difference in ESV intensity between north and south is obvious, and the southern part of Anhui province as a whole is the northern part. A substantial spatial negative correlation exists between ESV intensity and carbon emission intensity and obvious aggregation characteristics. The industrial resource-oriented cities of Huaibei, Maanshan, Huainan, and Anqing emerge as the primary carbon sources, contributing 60.72% to 71.98% of the total carbon emissions in Anhui Province. These findings offer valuable insights for Anhui Province to devise rational land use policies toward achieving low-carbon green development goals.