Recent work has shown that solid‐state ¹H and ³¹P MRI can provide detailed insight into bone matrix and mineral properties, thereby potentially enabling differentiation of osteoporosis from osteomalacia. However, ³¹P MRI of bone mineral is hampered by unfavorable relaxation properties. Hence, accurate knowledge of these properties is critical to optimizing MRI of bone phosphorus. In this work, ³¹P MRI signal‐to‐noise ratio (SNR) was predicted on the basis of T₁ and T₂* (effective transverse relaxation time) measured in lamb bone at six field strengths (1.5–11.7 T) and subsequently verified by 3D ultra‐short echo‐time and zero echo‐time imaging. Further, T₁ was measured in deuterium‐exchanged bone and partially demineralized bone. ³¹P T₂* was found to decrease from 220.3 ± 4.3 µs to 98.0 ± 1.4 µs from 1.5 to 11.7 T, and T₁ to increase from 12.8 ± 0.5 s to 97.3 ± 6.4 s. Deuteron substitution of exchangeable water showed that 76% of the ³¹P longitudinal relaxation rate is due to ¹H–³¹P dipolar interactions. Lastly, hypomineralization was found to decrease T₁, which may have implications for ³¹P MRI based mineralization density quantification. Despite the steep decrease in the T₂*/T₁ ratio, SNR should increase with field strength as B₀^0.4 for sample‐dominated noise and as B₀^1.1 for coil‐dominated noise. This was confirmed by imaging experiments. Copyright © 2013 John Wiley & Sons, Ltd.