In this work, we present the synthesis of a green‐emitting series of BaGd2ZnO5:xHo3+ (0.5–3 mol%) phosphors using a high‐temperature solid‐state reaction method. Phase purity and crystal structure information were evaluated through X‐ray powder diffraction patterns. Optical properties were examined through diffuse reflectance spectra, revealing that the prepared phosphor exhibited a band gap of 4.65 eV. The effect of Ho3+ doping on the morphology and ion distribution on the surface was assessed using scanning electron microscopy and time‐of‐flight secondary ion mass spectrometry techniques, respectively. The excitation spectra of the synthesized phosphor exhibited a charge transfer band and strong absorption transitions. The emission spectra displayed typical holmium emission characteristics, featuring a strong green emission band associated with f–f transitions from 5F4 + 2S2 → 5I8. Decay dynamics of the synthesized phosphor exhibited a single‐exponential decay pattern, with lifetimes ranging from 0.103 to 0.053 ms. The intrinsic radiative lifetime, calculated through Auzel's fitting was determined to be 0.14 ms. Using the emission spectra, colorimetric behaviour was analyzed, revealing that the Commission Internationale de l'éclairage (CIE) coordinates exclusively lay within the green region at (0.285, 0.705), with an impressive colour purity of 99.6%. Given these marked properties, the synthesized phosphor exhibits great potential for a wide range of green‐emitting applications, including displays, white light‐emitting diodes, and security signage.