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The present communication is strongly focused on the investigation of synthesis, structural and luminescence properties of cerium (Ce3+)‐ and europium (Eu3+)‐activated Zn4Al22O37 phosphors. Ce3+‐ and Eu3+‐doped Zn4Al22O37 novel phosphors were prepared using a solution combustion synthesis route. Structural properties were studied using powder X‐ray diffraction and high‐resolution transverse electron microscopy. The optical properties were studied using ultraviolet–visible light spectroscopy and Fourier transform infrared spectroscopy; luminescence properties were studied using a photoluminescence (PL) technique. The crystal structure of the prepared Zn4Al22O37 host and Ce3+‐ and Eu3+‐activated Zn4Al22O37 phosphors was investigated and was found to have a hexagonal structure. The measured PL emission spectrum of the Ce3+‐doped Zn4Al22O37 phosphor showed an intense and broad emission band centred at 421 nm under a 298 nm excitation wavelength. By contrast, the Eu3+‐doped Zn4Al22O37 phosphor exhibited two strong and intense emission bands at approximately 594 nm (orange) and 614 nm (red), which were monitored under 395 nm excitation. The Commission Internationale de l'Eclairage (CIE) colour coordinates of the Ce3+‐doped Zn4Al22O37 were investigated and found to be x = 0.1567, y = 0.0637 (blue) at 421 nm and for Eu3+‐doped Zn4Al22O37 were x = 0.6018, y = 0.3976 (orange) at 594 nm and x = 0.6779, y = 0.3219 (red) at 614 nm emission. The luminescence behaviour of the synthesized phosphors suggested that these phosphors may be used in lighting applications. [ABSTRACT FROM AUTHOR]