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