8 at.%, 10 at.%, and 12 at.% Dy3+ ions doped GdCa4O(BO3)3 crystals were successfully grown by the Czochralski method. The Raman spectrum showed that the maximum phonon energy was 937 cm−1. Detailed investigation of polarized absorption spectra, polarized fluorescence spectra, and fluorescence decay curve of the Dy3+:GCOB crystals showed that all the three crystals had good spectral properties. The strong and wide absorption peaks at 454 nm indicated that the crystals were fit for commercially available blue InGaN LD pumping. The intense and broad emission bands at around 585 nm, and long fluorescence lifetimes, revealed that the Dy3+:GCOB crystals were potential solid-state laser materials for yellow laser.