The advanced strategy of processing of NMR cross-polarization (CP) data has been developed separating the short-range order- and the bulk effects in the manifold of spin interactions. The effectiveness of such treatment have been demonstrated on 1H–31P CP kinetics in the nanostructured calcium hydroxyapatite (nano-CaHA) and that containing amorphous phosphate phase (amorph-CaHA). This allowed to describe the oscillatory manner of CP kinetics, oscillation blurring phenomenon, and to determine the spin distribution at the short- and moderate internuclear distances. The contribution of the dipolar coupling with remote spins has been removed modeling their spatial distribution using a set of radial profiles. The short 31P–1H contact peak at 0.24–0.27 nm has been well resolved in the spatial distribution profile of the nano-CaHA sample and it is hardly noticeable in the case of amorph-CaHA. It reflects the differences in surface organization in nanostructured and amorphous materials. The spin diffusion process...