Congenital abnormalities, trauma, and disease result in significant demands for bone replacement in the craniofacial region and across the body. Tetra-compositions of organic and inorganic scaffolds could provide advantages for bone regeneration. This research aimed to fabricate and characterize amorphous calcium phosphate (ACP)/calcium sulfate hemihydrate (CSH) with alginate/cellulose composite scaffolds using 3D printing. Alginate/cellulose gels were incorporated with 0%, 13%, 15%, 18%, 20%, and 23% ACP/CSH using the one-pot process to improve morphological, physiochemical, mechanical, and biological properties. SEM displayed multi-staggered filament layers with mean pore sizes from 298 to 377 μm. A profilometer revealed mean surface roughness values from 43 to 62 nm that were not statistically different. A universal test machine displayed the highest compressive strength and modulus with a statistical significance in the 20% CP/CS group. FTIR spectroscopy showed peaks in carbonate, phosphate, and sulfate groups that increased as more ACP/CSH was added. Zero percent of ACP/CSH showed the highest swelling and lowest remaining weight after degradation. The 23% ACP/CSH groups cracked after 60 days. In vitro biocompatibility testing used the mouse osteoblast-like cell line MC3T3-E1. The 18% and 20% ACP/CSH groups showed the highest cell proliferation on days five and seven. The 20% ACP/CSH was most suitable for bone cell regeneration.