Nanodiamonds with embedded nitrogen-vacancy (NV) centers have emerged as promising magnetic field sensors, as hyperpolarizing agents in biological environments, as well as efficient tools for spin mechanics with levitating particles. These applications currently suffer from random environmental interactions with the diamond which implies poor control of the N-V direction. Here, we predict and report on a strong diamagnetism of a pure spin origin mediated by a population inversion close to a level crossing in the NV center electronic ground state. We show control of the sign of the magnetic susceptibility as well as angle locking of the crystalline axis of a microdiamond along an external magnetic field, with bright perspectives for these applications.