A europium pyrosilicate, Eu2MgSi2O7 (1), is obtained using a high-temperature solid-state reaction. It crystallizes in the tetragonal noncentrosymmetric space group P4combining macron21m, and its structure features a 2D structure built by SiO4 and MgO4 tetrahedra, resulting in interlayer cavities occupied by Eu2+ ions. It has a SHG intensity around 0.7 times that of KTP in the particle size range of 45-75 μm under 2.1 μm radiation, demonstrating a relatively strong effect among the silicates. A typical photoluminescence phenomenon of Eu2+ can be observed at 482 nm. Calculations on the electronic structure and optical properties of 1 are performed. Moreover, to discuss the potential of pyrosilicates and related compounds as NLO crystals, the theoretical analysis on other A2BM2O7 compounds is also addressed.