We study spectral features of ion velocity and magnetic field correlations in the magnetosheath and in the solar wind using data from the Magnetospheric Multiscale (MMS) spacecraft. High-resolution MMS observations enable the study of the transition of these correlations between their magnetofluid character at larger scales into the subproton kinetic range, previously unstudied in spacecraft data. Cross-helicity, angular alignment, and energy partitioning is examined over a suitable range of scales, employing measurements based on the Taylor frozen-in approximation as well as direct two-spacecraft correlation measurements. The results demonstrate signatures of alignment at large scales. As kinetic scales are approached, the alignment between v and b is destroyed by demagnetization of protons.