Skarns are residue of relatively low-temperature magma-induced decarbonation in the crust largely associated with silicic plutons. Mafic magmatic intrusions are also capable of releasing excess CO2 due to carbonate assimilation. However, the effect of mafic to silicic melt evolution on the decarbonation processes, in addition to temperature controls on carbonate-intrusive magmatic systems, particularly at continental arcs, remains unclear. In this study, experiments performed in a piston cylinder apparatus at midcrustal depth (0.5 GPa) at supersolidus temperatures (900–1200°C) document calcite interaction with andesite and dacite melts at equilibrium under closed-system conditions at calcite saturation in a 1:1 melt-calcite ratio by weight. With increasing silica content in the starting melt, at similar melt fractions and identical pressure, assimilation decreases drastically (≤65% andesite-calcite to ≤18% dacite-calcite). In conjunction, the CaO/SiO2 ratio in melts resulting from calcite assimilation in andesitic starting material is >1, but ≤0.3 in those formed from dacite-calcite interaction. With increasing silica-content in the starting melt skarn mineralogy, particularly wollastonite, increases in modal abundance while diopsidic clinopyroxene decreases slightly. More CO2 is released with andesite-calcite reaction (≤2.9 × 1011 g/y) than with more skarn-like dacite-calcite interaction (≤8.1 × 1010 g/y, at one volcano assuming respective calcite-free-superliquidus conditions and a magma flux of 1012 g/y). Our experimental results thus suggest that calcite assimilation in more mafic magmas may have first degassed a significant amount of crustal carbon before the melt evolves to more silicic compositions, producing skarn. Crustal decarbonation in long-lived magmatic systems may hence deliver significant albeit diminishing amounts of carbon to the atmosphere and contribute to long-term climate change.