To realize quantum information processing, quantum bits are required to have considerable quantum coherence, addressability, and scalability. Arranging and stacking of the high dimensional quantum bits which have superior coherence is an important approach to realize the scalability of the quantum systems. Endohedral nitrogen fullerene is a promising molecule-based quantum material with long quantum coherence time, which is expected to apply to the construction of high-dimensional quantum bit arrays for quantum information processing. In this work, endohedral nitrogen fullerene molecules were embedded in 3D metal−organic framework yielding N@C60@MOF-177. X-band electron paramagnetic characterization of the energy levels and spin dynamics shows that this system can be used as spin qubit. The magnitude of the zero-field splitting of the system at low temperature was properly resolved. Furthermore, the influence factors on the spin coherence time at low temperature are investigated by spin dynamic characterization and the presence of the proton in the environment is detected by ESEEM experiments,which further reveals the feasibility of N@C60 as a spin quantum sensor.