To stabilize nontrivial spin textures, e.g., skyrmions or chiral domain walls in ultrathin magnetic films, an additional degree of freedom, such as the interfacial Dzyaloshinskii-Moriya interaction (IDMI), must be induced by the strong spin-orbit coupling (SOC) of a stacked heavy metal layer. However, advanced approaches to simultaneously control the IDMI and perpendicular magnetic anisotropy (PMA) are needed for future spin-orbitronic device implementations. Here, we show the effect of atomic-scale surface modulation on the magnetic properties and IDMI in ultrathin films composed of 5d heavy metal/ferromagnet/4d(5d) heavy metal or oxide interfaces, such as Pt/CoFeSiB/Ru, Pt/CoFeSiB/ Ta, and Pt/CoFeSiB/MgO. The maximum IDMI value corresponds to the correlated roughness of the bottom and top interfaces of the ferromagnetic layer. The proposed approach for significant enhancement of PMA and the IDMI through interface roughness engineering at the atomic scale offers a powerful tool for the development of spinorbitronic devices with precise and reliable controllability of their functionality.