This paper presents a comprehensive study on thermal, structural and optical properties of novel willemite glass-ceramics. The precursor glass in the ZnO-SLS glass system was successfully prepared using conventional meltquenching technique and willemite (Zn 2 SiO 4 ) glass-ceramics were derived from this precursor glass by a control crystallization process. The effect of heat-treatment temperature on the phase transformation, morphology and size of Zn 2 SiO 4 crystal phase was examined using X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM) techniques. Furthermore, fourier transform infrared reflection (FTIR) spectroscopy was used to evaluate the Zn 2 SiO 4 crystal structural evolution. The average size of Zn 2 SiO 4 crystallite obtained from calculation of XRD is found to be in the range 30-60 nm, whereas the grain size observed in FESEM is in range of 200-400 nm. The appearance of SiO 2 , ZnO 4 and Zn-O-Si bands detected from FTIR indicate the formation of Zn 2 SiO 4 crystal phase. Besides, the study of the optical band gap has found that optical band gap of the glass-ceramics decreased as the heat treatment temperature increased. The photoluminescence spectra of willemite glass-ceramics exhibit two different emissions around 525 nm (green) and 585 nm (yellow); exhibit a characteristic of broad absorption band around 260 nm. These two different spectra reveal that the luminescence performance of the willemite glass-ceramics was enhanced with the progression of heat treatment temperature due to different located energy levels of the b-Zn 2 SiO 4 and a-Zn 2 SiO 4 crystalline phase. Such luminescent glass-ceramics was expected to find potential applications in phosphors and opto-electronic devices.