The structural and magnetic properties of the square-cupola antiferromagnet Sr(TiO)Cu4(PO4)4 are investigated via x-ray diffraction, magnetization, heat capacity, and 31 P nuclear magnetic resonance experiments on polycrystalline samples, as well as density-functional band-structure calculations. The temperature-dependent unit cell volume could be described well using the Debye approximation with the Debye temperature of θD 550 K. Magnetic response reveals a pronounced two-dimensionality with a magnetic long-range-order below TN 6.2 K. High-field magnetization exhibits a kink at 1/3 of the saturation magnetization. Asymmetric 31 P NMR spectra clearly suggest strong in-plane anisotropy in the magnetic susceptibility, as anticipated from the crystal structure. From the 31 P NMR shift vs bulk susceptibility plot, the isotropic and axial parts of the hyperfine coupling between 31 P nuclei and the Cu 2+ spins are calculated to be A iso hf 6539 and A ax hf 952 Oe/µB, respectively. The low-temperature and low-field 31 P NMR spectra indicate a commensurate antiferromagnetic ordering. Frustrated nature of the compound is inferred from the temperature-dependent 31 P NMR spin-lattice relaxation rate and confirmed by our microscopic analysis that reveals strong frustration of the square cupola by next-nearest-neighbor exchange couplings.