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Converting biowaste into biochar and incorporating it into soil is recognized as an effective method for carbon (C) sequestration. However, biochar inevitably undergoes an aging process in soil, which influences its stability, and ultimately threatens its carbon sequestration ability. This study selected CaCl2 as an exogenous additive of sewage sludge and bone dreg for producing Ca-rich biochars, and both surface C and bulk C stability in them were investigated under three aging processes (dry–wet aging, freeze–thaw aging, and natural aging in farmland soil). The results showed that the above three aging processes resulted in oxidized surface C in Ca-rich biochar decreasing by 10~23%, 28~41%, and 0~74%, respectively, compared with that in pristine biochar, while oxidized bulk C decreased by 6~10%, 0~1%, and 0~35%, respectively. This was attributed to the “protective effect” of Ca-containing crystals on the biochar surface, including CaO, Ca5(PO4)3Cl, Ca5(PO4)3(OH), Ca8H2(PO4)6·H2O, and Ca10(PO4)6(OH)2, which intervened in the oxidation of C–C/C=C in biochar but also reduced the generation of a fragmented C structure. By comprehensively assessing surface C and bulk C stability under three aging processes, final C sequestration in Ca-rich biochar increased to 27~80%, compared to that in pristine biochar (23~74%). Therefore, Ca-rich biochar is more dominant than pristine biochar, considering C sequestration potential during long-term aging in soil.