Calcium phosphate cement (CPC) has superior properties, such as excellent bioactivity, biocompatibility, osteoconductivity and degradability, since its hydration product is hydroxyapatite (HA). As a novel cement material, CPC also shows injectable and self-setting properties. However, the compressive strength (CS) and fracture toughness of most CPCs are far lower than that of human weight-bearing bones, which largely limit their applications in the repairment of weight-bearing bones. To improve the CS and fracture toughness of CPC, several methods, including in-situ reinforcement by Ca4(PO4)2O (TTCP) ceramic particles, suitable nanofibers are introduced in this study. The maximal CS of CPC prepared with TTCP (average particle size of 22.3 ± 0.4 μm) reached to 98.4 MPa, which is close to the strength of human long bones. The enhanced CS of CPC was attributed to the in-situ reinforcing effect of residual TTCP particles. Tendon collagen slices and HA nanofibers were used to improve the fracture toughness of CPC. The flexural strength (FS) and the work of facture (WOF) of CPC were slightly increased by adding HA nanofibers but was significantly increased by the addition of tendon collagen slices. With 1.000 wt% tendon collagen slices, the FS and WOF of CPC were increased by 61.3% and 22.6 times, respectively.