Disordered crystals have attracted immense attention for the generation of ultrashort laser pulses due to their good thermomechanical characteristics and wide emission bandwidths. In this work, a Gd-based orthophosphate crystal, GdSr3(PO4)3, (GSP), and a Nd3+-doped GdSr3(PO4)3 crystal, (Nd:GSP), were obtained by the Czochralski method. The crystal structure, optical properties, electronic band structure, laser damage threshold, and hardness of the GSP crystal were comprehensively investigated. It exhibited a disordered structure due to the random distribution of Sr and Gd atoms in the same Wyckoff site, which caused inhomogeneous spectral broadening. Additionally, it exhibited a short UV absorption cutoff edge (<200 nm), a large band gap (5.81 eV), and a high laser damage threshold (∼1850 MW/cm2). The spectral properties and Judd-Ofelt calculations of the Nd:GSP crystals were analyzed. A wide absorption band at 803 nm, with a full width at half-maximum value of 20 nm, makes the Nd:GSP crystal suitable for the efficient pumping of AlGaAs laser diodes. Sub-100-fs pulses could be supported by its 25 nm emission bandwidth. Hence, the GSP crystal could be a promising disordered crystal laser matrix.