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Developing multimodal contrast agents is an upcoming area and hydroxyapatite nanoparticles substituted with various elements like gadolinium, eurobium etc., seems to be a promising contrast agent, especially for multimodal imaging of bone-tissue interface. A bimodal contrast agent using silver (Ag+) and gadolinium (Gd3+) ions co-substituted hydroxyapatite nanoparticles has been developed for X-ray and magnetic resonance imaging. Ag+ and Gd3+ ions were co-substituted into hydroxyapatite at various atomic percentages (Ag:Gd=0.25:0.25, 0.25:0.5, 0.25:0.75) using microwave accelerated wet chemical synthesis. Pure as well as Ag+ and Gd3+ ions substituted hydroxyapatite samples were also synthesized for comparison. All samples were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy etc., and found to be monophasic, nanocrystalline with the substituted ions. These co-substituted hydroxyapatite samples were then tested in different diagnostic modalities such as X-ray, computed tomography imaging and magnetic resonance imaging. Appreciable variation in contrast was observed with different amount of substitutions. All the Ag+ and Gd3+ ions co-substituted hydroxyapatite nanoparticles showed higher contrast in all imaging modalities compared to those substituted with either Ag+ or Gd3+ ions only. Hydroxyapatite sample co-substituted with 0.25Ag and 0.75Gd at. % substitution showed the best bimodal CT-MRI contrast.