Calcium aluminate cement (CAC)—based strain hardening cementitious composites (SHCC) has been developed and used for the rehabilitation of sewerage pipelines. In addition to well-known microbiologically induced corrosion, CO2 concentration in the sewerage environment is high, which may cause significant carbonation of pipelines. Thus, this paper aims to investigate the effects of carbonation on the mechanical performance of CAC-based SHCC. Two types of CAC-based SHCC with different strength grades and a referenced OPC-based SHCC were prepared. The accelerated carbonation test was conducted in a carbonation chamber with a 5% CO2 concentration. The compressive and tensile behaviour of SHCC was tested first, and microstructure analysis, e.g., X-ray diffraction and scanning electron microscopy, was then performed. The results showed that CAC-based SHCC specimens exhibited robust strain-hardening performance as well as large deformation capacity in tension due to the fiber-bridging effect. Also, the compressive and tensile strength was significantly improved as well as achieving a higher tensile strain capacity after carbonation when compared with OPC-based SHCC. Microstructure analysis revealed that the metastable phases in carbonated CAC-based SHCC were converted into stable phases and calcium carbonate polymorphs, densifying the binder matrix. The obtained results of this paper may provide new insight into utilizing carbonation to avoid the unstable conversion of hydrates in calcium aluminate cement.