We report the formation of perfectly aligned, high-density, shallow nitrogen vacancy (NV) centers on the Perfectly aligned shallow ensemble NV centers indicated a high Rabi contrast of approximately 30 % which is comparable to the values reported for a single NV center. Nanoscale NMR demonstrated surfacesensitive nuclear spin detection and provided a confirmation of the NV centers depth. Single NV center approximation indicated that the depth of the NV centers was approximately 9-10.7 nm from the surface with error of less than ±0.8 nm. Thus, a route for material control of shallow NV centers has been developed by step-flow growth using a CVD system. Our finding pioneers on the atomic level control of NV center alignment for large area quantum magnetometry. 6,7 . A fundamental limitation of an NV center based magnetometer is the material control required to confine the NV center in the vicinity (<10 nm) of the substrate surface with a high magnetic sensitivity.Previous studies that examined shallow NV centers focused on either a high-density ensemble for twodimensional large area imaging or a single NV center for high contrast and high coherent time to obtain a minimal detection volume using nanoscale NMR. However, it was found necessary to combine spatial localization of a NV centers with alignment, high density, and a long spin coherence time (T2) to obtain high magnetic sensitivity. The alignment of NV centers in an ensemble is the key to accomplish high contrast while maintaining high signal to noise ratio for high magnetic sensitivity with low accumulation time. In this regard, low energy ion implantation is the most common technique utilized for the production of NV centers in the vicinity of a surface 8 . However, this methodology suffers from large depth dispersion (>10 nm) of the NV centers due to ion straggling and channeling effects 9,10 . Additionally, high-density surface defects formed during implantation affect the spin coherence time and the ensembles show a random orientation with this technique 12,13,14 . Existing studies include reports of CVD growth that demonstrated a narrow distribution in the confinement of NV centers in the vicinity of a surface 11 and their atomic alignment on (100), (110), (113), and (111) substrates for the formation of thick diamond films 14,15,16,17,18,19,20 . Nearly all previous studies have focused on either low density NV centers (<10 13 cm -3 3 ) in the vicinity of a surface with no alignment 21,22,23 or the formation of NV ensembles with alignment in bulk.In this paper, the formation of a perfectly aligned high-density shallow NV center film for surfacesensitive detection of nuclear spin has been demonstrated. Results obtained from SIMS measurement combined with an effective depth obtained from nanoscale NMR measurement confirms presence of shallow NV center approximately 9-10.7 nm from surface with error of less than ±0.8 nm. The results of this study offer a path toward controlling the alignment of shallow NV center ensembles.In this study, NV-containing d...