To compensate the limitations of bone tissue magnetic resonance imaging (MRI), a series of gadolinium (Gd ) substituted β-Tricalcium phosphate [β-TCP, β-Ca (PO ) ] were developed. All the powders were characterized using XRD, Raman spectroscopy, Rietveld refinement of the XRD data and the studies confirmed the Gd occupancy at Ca (1), Ca (2) and Ca (3) lattice sites of β-Ca (PO ) HR-TEM analysis revealed the spherical nature of particles with diameter about 100 nm. The Gd doped β-Ca (PO ) exhibited non-toxic behaviour to MG-63 cells in vitro and the room temperature magnetic field versus magnetization measurements confirmed its paramagnetic behaviour. MRI analysis revelas that it shorten both T and T proton relaxation times, thus influencing both r and r relaxivity values that reach 61.97 mM s and 73.35 mM s . © 2016 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 105B: 2545-2552, 2017.