Mn–Cu‐based alloys possess excellent mechanical and functional properties (damping capacity and shape memory effect). This work utilizes a typical additive manufacturing technique, selective laser melting (SLM), to fabricate Mn–15 wt%Cu alloys to explore the mechanical and functional behaviors. The results indicate that the γ‐(Mn, Cu) and a small amount of γ′‐(Mn, Cu) phase are the main phase compositions in the as‐SLMed Mn–15 wt%Cu alloy, as well as twins and second‐phase precipitation particles. The microstructure shows a fine cellular γ‐(Mn, Cu) dendrite with primary dendrite spacing of ≈0.9 μm in the columnar grains with a size of ≈8 μm. The martensitic transformation start temperature (MS) and phase transformation hysteresis are ≈132.6 and ≈5.1 °C, respectively. The existing nanoscale chemical segregations of Mn and Cu are attributed to the spinodal decomposition of γ‐(Mn, Cu). A compositional modulation is observed with a wavelength of ≈20 nm and an amplitude fluctuation of Mn (55–85 wt%) and Cu concentrations (15–45 wt%). Finally, the as‐SLMed Mn–15 wt%Cu alloy boasts good tensile properties (359, 268 MPa, and 3.6%), damping (internal friction of 0.032 when the strain amplitude is 9 × 10−4), and shape memory performances (one‐way ηow = 37–48%, and two‐way ηtw = 16–20% under the pre‐deformation strain of 2–3%).