We report on detailed studies of electronic and nuclear spin states in the diamond-nitrogen-vacancy (NV) center under weak transverse magnetic fields. We numerically predict and experimentally verify a previously unobserved NV hyperfine level anticrossing (LAC) occurring at bias fields of tens of gauss-two orders of magnitude lower than previously reported LACs at ∼500 and ∼1000 G axial magnetic fields. We then discuss how the NV ground-state Hamiltonian can be manipulated in this regime to tailor the NV's sensitivity to environmental factors and to map into the nuclear spin state. DOI: 10.1103/PhysRevA.94.021401 Nitrogen-vacancy (NV) defect centers in diamond are optically polarizable quantum systems with spin-dependent fluorescence. Using electron spin resonance (ESR) under ambient conditions, sensitivity to electric fields [1][2][3][4], transverse and axial magnetic fields [5][6][7][8][9][10], temperature [11][12][13][14], strain [15], and pressure [16] have been observed via resonance frequency shifts of the NV ground-state manifold. Nonseparable sensitivity to multiple environmental factors is problematic when it comes to using the NV as a sensor. However, the Hamiltonian governing the measurable frequency shifts can be tailored to enhance (or to suppress) sensitivity to different physical phenomena. A magnetic bias field applied parallel or perpendicular [B || or B ⊥ as shown in Fig. 1(a)] to the NV's axis in the diamond crystal lattice energetically separates the spin states and increases sensitivity to magnetic or electric fields, respectively.In this Rapid Communication, we investigate an unexplored weak-field regime in which electronic spin ground-state energy level splittings are on par with the Zeeman shift induced by an applied magnetic field. Here we account for both the electron and the nuclear spin of the NV, which reveals complex dynamics of nuclear spin state degeneracy and previously unobserved hyperfine level anticrossings. These features occur at a low magnetic field (B ⊥ 40 G) as compared to the B || ∼ 500 and B || ∼ 1000 G excited-and ground-state crossings [17][18][19][20], which have been used for nuclear spin polarization, providing increased sensitivity to resonance shifts through narrower effective linewidth and increased contrast [21][22][23][24]. We find excellent agreement between experiment and theory and discuss the utility of the nuclear spin degeneracy regime toward NV sensing applications and solid-state atomic memories based on nuclear spin polarization. While the results described here are specific to the NV, similar anticrossings are expected in any spin-1 (or higher) defect center that shows hyperfine level splitting on the same order of magnitude as double-electron spin flip anticrossings.The NV is a two-site defect with a spin-1 electronic ground state, which is magnetically coupled to nearby nuclear spins.For a single NV orientation, energy level shifts are described by the following spin Hamiltonian of the ground triplet state in the presence of magnetic, electric, ...