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Materials based on highly reactive α-tricalcium phosphate (α-TCP) powder were developed and evaluated. Furthermore, the impact of different polymeric additives, such as citrus pectin or polyacrylamide (PAAM) modified with sago starch, neem flower, or rambutan peel, on the physiochemical and biological properties of the developed materials was assessed. The addition of modified PAAM shortened the setting process of bone cements and decreased their compressive strength. On the other hand, the addition of citrus pectin significantly enhanced the mechanical strength of the material from 4.46 to 7.15 MPa. The improved mechanical properties of the bone cement containing citrus pectin were attributed to the better homogenization of cementitious pastes and pectin cross-linking by Ca2+ ions. In vitro tests performed on L929 cells showed that 10% extracts from α-TCP cements modified with pectin are more cytocompatible than control cements without any additives. Cements containing PAAM with plant-derived modifiers show some degree of cytotoxicity for the highly concentrated 10% extracts, but for diluted extracts, cytotoxicity was reduced, as shown by a resazurin reduction test and live/dead staining. All the developed bone substitutes exhibited in vitro bioactivity, making them promising candidates for further biological studies. This research underscores the advantageous properties of the obtained biomaterials and paves the way for subsequent more advanced in vitro and in vivo investigations. [ABSTRACT FROM AUTHOR]