Global warming linked to the industrial emissions of greenhouse gases may be the end of mankind unless it is adequately and timely handled. To prevent irreversible changes to the climate of the Earth, numerous research groups are striving to develop robust CO2 sorbents. Dialkyl carbonates (DACs) and CO2 exhibit obvious chemical similarities in their structure and properties. The degrees of oxidation of all atoms composing DACs and CO2 are identical resulting in very similar nucleophilicities and electrophilicities of all interaction centers. While both compounds possess relatively high partial atomic charges on their polar moieties, the molecular geometries prevent tight binding of the head groups. The computed DAC-DAC binding energies are ∼40 kJ mol-1, whereas the effect of the alkyl chain length is marginal. The phase transition points and shear viscosities of DACs are very low. We herein hypothesize and numerically rationalize that DACs represent noteworthy physical sorbents for CO2 thanks to the similar sorbent-CO2 and sorbent-sorbent interaction energies. By reporting in silico-derived sorption thermodynamics at various conditions, spectral and structural properties, and experimentally derived CO2 capacities and recyclabilities, we highlight the mutual affinity of DACs and CO2. Indeed, the experimentally determined CO2 sorption capacity of 0.88 mol% (diethyl carbonate) at 278.15 K and 30 bar is competitive. The unprecedentedly low DAC-CO2 binding energies, ∼14 kJ mol-1, suggest a low-cost desorption process and outstanding recyclability of the sorbent. We also note that DACs possessing long alkyl chains (butyl, hexyl, octyl) exhibit negligible volatilities, while preserving the liquid aggregate state over a practically important temperature range. The reported results may foster the development of a new class of CO2 scavengers with possibly quite peculiar characteristics.