Background: The standard MR Dixon-based attenuation correction (AC) method in Positron Emission Tomography / Magnetic Resonance (PET/MR) imaging segments only the air, lung, fat and soft-tissues (4-class), thus neglecting the highly attenuating bone tissues and affecting quantification in bones and adjacent vessels. We sought to address this limitation by utilizing the distinctively high bone uptake rate constant Ki expected from 18 F-Sodium Fluoride (18 F-NaF) to segment bones from PET data and support 5-class hybrid PET/MR-driven AC for 18 F-NaF and 18 F-Fluorodeoxyglucose (18 F-FDG) PET/MR cardiovascular imaging. Methods: We introduce 5-class Ki/MR-AC for (i) 18 F-NaF studies where the bones are segmented from Patlak Ki images and added as the 5 th tissue class to the MR-Dixon 4-class AC map. Furthermore, we propose two alternative dual-tracer protocols to permit 5-class Ki/MR-AC for (ii) 18 F-FDG-only data, with a streamlined simultaneous administration of 18 F-FDG and 18 F-NaF at 4:1 ratio (R4:1), or (iii) for 18 F-FDG-only or both 18 F-FDG and 18 F-NaF dual-tracer data, by administering 18 F-NaF 90 min after an equal 18 F-FDG dosage (R1:1). The Ki-driven bone segmentation was validated against Computed Tomography (CT)-based segmentation in rabbits, followed by PET/MR validation on 108 vertebral bone and carotid wall regions in 16 human volunteers with and without prior indication of carotid atherosclerosis disease (CAD). Results: In rabbits, we observed similar (<1.2% mean difference) vertebral bone 18 F-NaF SUVmean scores when applying 5-class AC with Ki-segmented bone (5-class Ki/CT-AC) versus CT-segmented bone (5-class CT-AC) tissue. Considering the PET data corrected with continuous CT-AC maps as gold-standard, the percentage SUVmean bias was reduced by 17.6% (18 F-NaF) and 15.4% (R4:1) with 5-class Ki/CT-AC versus 4-class CT-AC. In humans without prior CAD indication, we reported 17.7% and 20% higher 18 F-NaF target-to-background ratio (TBR) at carotid bifurcations wall and vertebral bones, respectively, with 5-versus 4-class AC. In the R4:1 human cohort, the mean 18 F-FDG TBR increased by 12.2% at carotid bifurcations wall and 19.9% at vertebral bones. For the R1:1 cohort of human without CAD indication, mean TBR increased by 15.3% (18 F-FDG) and 15.5% (18 F-NaF) at carotid bifurcations and 21.6% (18 F-FDG) and 22.5% (18 F-NaF) at vertebral bones. Similar TBR enhancements were observed whe applying the proposed AC method to human subjects with prior CAD indication.. Conclusions: Ki-driven bone segmentation and 5-class hybrid PET/MR-driven AC is feasible and can significantly enhance 18 F-NaF and 18 F-FDG contrast and quantification in bone tissues and carotid walls.