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Vitreous substitutes are crucial adjuncts during vitreo-retinal surgery for retinal diseases such as complicated retinal detachment, macular holes, complications of diabetic retinopathy, and ocular trauma involving posterior segment. In retinal detachment surgery, an internal tamponade agent is required to provide internal pressure for reattachment of the detached neurosensory retina. Current available options serve only as a temporary surgical adduct or short-term solution and are associated with inherent problems. Despite many years of intensive research, an ideal vitreous substitute remains elusive. Indeed, the development of an ideal vitreous substitute requires the concerted efforts of synthetic chemists and biomaterial engineers, as well as ophthalmic surgeons. In this review, we propose that polymeric hydrogels present the future of artificial vitreous substitutes due to its high water composition, optical transparency, and rheological properties that closely mimic the natural vitreous. In particular, thermosensitive smart hydrogels, with reversible sol to gel change, have emerged as the material class with the most potential to succeed as ideal vitreous substitutes, facilitating easy implementation during surgery. Importantly, these smart hydrogels also display potential as efficacious drug delivery systems.