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Regolith carbonates are common in soil profiles in the arid to semiarid areas of southern and central Australia. Extrinsic sources are now inferred to be the dominant source of Ca even as far inland as Alice Springs in central Australia. This study of Ca sources in a near coastal 2 m deep profile at Clarendon, South Australia, and two inland 4- and 3 m-deep profiles near Olary, South Australia uses Sr isotopes as a proxy for Ca. Our results show that up to 90% of Sr (and by association Ca) in both labile fractions and in soil carbonate is sourced from atmospheric input. The silicate weathering input is minor (<10%) and independent of the influence of different bedrock types. The Sr isotope composition throughout the profiles is relatively homogeneous with most values between 0.714 and 0.717, increasing only when in the saprolith, indicating that a process of continual reworking and mixing of the Sr (and Ca) goes beyond the near surface and continues throughout the profile.