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Abstract We investigated the state of the arc background mantle (i.e. mantle wedge without slab component) by means of olivine CaO and its Cr-spinel inclusions in a series of high-Mg# volcanic rocks from the Quaternary Trans-Mexican Volcanic Belt. Olivine CaO was paired with the Cr# [molar Cr/(Cr + Al) *100] of Cr-spinel inclusions, and 337 olivine+Cr-spinel pairs were obtained from 33 calc-alkaline, high-K and OIB-type arc front volcanic rocks, and three monogenetic rear-arc basalts that lack subduction signatures. Olivine+Cr-spinels display coherent elemental and He–O isotopic systematics that contrast with the compositional diversity of the bulk rocks. All arc front olivines have low CaO (0.135 ± 0.029 wt %) relative to rear-arc olivines which have the higher CaO (0.248 ± 0.028 wt %) of olivines from mid-ocean ridge basalts. Olivine 3He/4He–δ18O isotope systematics confirm that the olivine+Cr-spinels are not, or negligibly, affected by crustal basement contamination, and thus preserve compositional characteristics of primary arc magmas. Variations in melt H2O contents in the arc front series and the decoupling of olivine CaO and Ni are inconsistent with controls on the olivine CaO by melt water and/or secondary mantle pyroxenites. Instead, we propose that low olivine CaO reflects the typical low melt CaO of high-Mg# arc magmas erupting through thick crust. We interpret the inverse correlation of olivine CaO and Cr-spinel Cr# over a broad range of Cr# (~10–70) as co-variations of CaO, Al and Cr of their (near) primary host melts, which derived from a mantle that has been variably depleted by slab-flux driven serial melt extraction. Our results obviate the need for advecting depleted residual mantle from rear- and back-arc region, but do not upset the larger underlying global variations of melt CaO high-Mg# arc magmas worldwide, despite leading to considerable regional variations of melt CaO at the arc front of the Trans-Mexican Volcanic Belt.