This work reports on a new methodology for synthesizing poly(propylene fumarate) (PPF)/titania nanowire composites which would be beneficial in tissue engineering for orthopaedic bone cements. The synthetic procedure reacted PPF with maleic anhydride to create HOOC-PPF-COOH species in a ring-opening reaction at room temperature. These species were then coordinated to titania nanowires by metal carboxylate bonding through the end -COOH groups. These PPF-grafted nano-TiO2 assemblies were then further polymerized and crosslinked in the presence of N-vinylpyrrolidone to produce the bone cements. The synthesis and modification of PPF was confirmed by NMR (1H and 13C) and XPS, while the reaction chemistry of the functionalized PPF and nano-TiO2 was also investigated by XPS and FTIR. Mechanical testing of the resulting composites demonstrated a significant reinforcement of the tensile and flexural properties, showing the utility of this synthetic approach for bone tissue engineering.