A series of Dysprosium (Dy3+) doped -Tricalcium phosphate [-TCP, -Ca-3(PO4)(2)] were developed for applications in magnetic resonance imaging (MRI) and computed tomography (CT). Characterization studies confirmed the Dy3+ occupancy at Ca2+(1), Ca2+(2), and Ca2+(3) lattice sites of -Ca-3(PO4)(2) and its substitution limit was determined as 4.35mol%. The transitions from the H-6(15/2) ground state to various excited energy levels is validated by the characteristic absorption peaks of Dy3+. Luminescence studies inferred two intense bands at 480 and 572nm due to (F9/2H15/2)-F-4-H-6 (blue) and (F9/2H13/2)-F-4-H-6 (yellow) transitions of Dy3+. The paramagnetic and nontoxic behavior of Dy3+-doped -Ca-3(PO4)(2) were confirmed from magnetic and MTT tests, respectively. Dy3+ in the host induces a high X-ray absorption ability for X-ray computed tomography (CT) and showed efficient contrast T-2-enhancing modality. Thus the proposed system could be used as a promising probe for multimodality with optical imaging, computed tomography and magnetic resonance imaging.