The loss of craniofacial tissue due to congenital and developmental conditions can lead to various negative impacts such as aesthetic, functional, and physiological aspects of one’s life. Conventional reconstruction methods have been characterized by limited availability, risk of resorption, and immune reaction. Advances in tissue engineering, including the fabrication of biomaterials, have been developed to overcome these challenges and allow the reconstruction and long-term rehabilitation of craniofacial defects. This task is complicated and time-consuming, owing to the intricate nature of the craniofacial region, which includes both highly vascularized and innervated soft and hard tissues with varying growth rates. Although some of these biomaterials are well-developed, their sustainability is often overlooked and is rarely the topic of discussion. Recently, greater attention has been placed on green development within tissue engineering, leading to a more prominent emphasis on the production of sustainable scaffolding materials. Here, we aim to discuss different sustainability concepts, as well as review current examples of sustainable biomaterials including synthetic materials such as PEEK, PEG, PLGA and natural-derived materials such as alginate, chitosan, and soy protein used in scaffolding therapies. The clinical applications of these materials for craniofacial tissue regeneration are also overviewed.