The aim of this research is to assess the influence of Sn inclusion on the microstructure evolution and age-hardening response of a Zn-4Cu alloy. This is the first study to correlate the age-hardening response to the microstructure of Zn-4Cu alloy reinforced with different Sn contents. A series of Zn-4Cu-Sn alloys were successfully fabricated with different Sn concentrations in the range of 0.0–4.0 wt.% using permanent mold casting. The microstructure of Zn-4Cu-Sn alloys was investigated by means of a scanning electron microscope (SEM) attached with an energy dispersive spectroscope (EDS) and X-ray diffraction (XRD) line profile analysis. At room temperature, the Vickers microhardness measurements were used to assess the age-hardening response of alloys. The results show that the microhardness of the Zn-4Cu (ZC) binary alloy increases a little bit from 76 to 80 HV as the aging time increases from 2 to 128 h, respectively. For aging times up to 16 h, the microhardness of all Sn-containing alloys decreases but then increases again. The lowest hardness belongs to the ZC-1.5Sn alloy, and the Sn-Zn-3.0Sn alloy has the highest; the other alloys fall somewhere in between. At high aging times (64 and 128 h), the microhardness of all Sn-containing samples increased continuously with an increasing Sn content from 0.0 to 3.0 wt.%. When the Sn-containing alloys (3.5 and 4.0 wt.% Sn) were aged for 64 and 128 h, the hardness declined by 7.94% and 8.90% compared to their peak aging hardness values, respectively. By considering the structural changes that occur in the Zn-4Cu-Sn alloys, the reasons for the observed variations in microhardness data with increasing Sn content and aging time were elucidated. X-ray diffraction (XRD) data was analyzed to determine the zinc matrix’s lattice parameters, c/a ratio, and unit cell volume variations.