To better meet the needs of modern science and technology for new inorganic functional materials, the exploration of new Eu2+-doped phosphors is of great significance. In this work, a zirconium-silicate yellow phosphor, K2ZrSiO5:Eu2+, was explored through theoretical calculations and systematic experiments for use in multifunctional applications. The crystal structure, electronic structure, photoluminescence (PL) and cathodoluminescence (CL) properties of K2ZrSiO5:Eu2+ were investigated in detail. As a result, owing to the open framework and the lattice with the covalent connection, K2ZrSiO5:Eu2+ phosphor exhibits strong yellow light emission under the near-ultraviolet and electron beam excitation. However, the K2ZrSiO5:Eu2+ phosphor suffers a poor thermal stability. Furthermore, the K2ZrSiO5:Eu2+ phosphor exhibits good anti-saturation and anti-aging characteristics under the electron beam excitation. The results indicate that the development of K2ZrSiO5:Eu2+ phosphor can provide a new insight into discovering multifunctional materials.