Carbon dioxide (CO2) is released from the Earth’s interior into the atmosphere through both volcanic and non-volcanic sources in a variety of tectonic settings. A quantitative understanding of CO2 outgassing fluxes in different geological settings is thus critical for decoding the link between the global carbon budget and different natural processes (e.g., volcanic eruption and earthquake nucleation) and the effects on the climate evolution over geological time. It has recently been proposed that CO2 degassing from non-volcanic areas is a major component of the natural CO2 emission budget, but available data are still sparse and incomplete. Here, we report the results of a geochemical survey aimed at quantifying CO2 emissions through cold and thermal springs of the tectonically active Pollino Massif and Calabrian arc (Southern Italy). The chemical ad isotopic (He and C) composition of fifty-five dissolved gas samples allows to identify two different domains: 1) a shallow system dominated by gas components of atmospheric signature (helium, hereafter He) and biogenic origin (C), and 2) a deeper system in which crustal/deep fluids (CO2 and He) are dominant. The measured He isotope ratios range from 0.03 to 1.1 Ra (where Ra is the He isotopic ratio in the atmosphere) revealing a variable atmospheric contamination. Furthermore, the He isotopic data indicate the presence of traces of mantle He contributions (2%–3%) in the thermal groundwater. The prevailing low R/Ra values reflect the addition of crustal radiogenic 4He during groundwater circulation. Using helium and carbon isotope data, we explore the possible sources of fluids and the secondary processes (dissolution/precipitation) that act to modify the chemistry of pristine volatiles. For the thermal springs, we estimate a deep C output of 2.3 x 107 to 6.1 x 108 mol year−1. These values correspond to deep CO2 fluxes per square km comparable with those estimated in several active and inactive volcanic areas and in continental regions affected by metamorphic CO2 degassing (e.g., the southern margin of the Tibetan Plateau).