An ensemble of nitrogen-vacancy (NV) centers in diamond is an attractive device to detect small magnetic fields. In particular, by exploiting the fact that the NV center can be aligned along one of four different axes due to C3ν symmetry, it is possible to extract information concerning vector magnetic fields. However, in the conventional scheme, low readout contrasts of the NV centers significantly decrease the sensitivity of the vector magnetic field sensing. Here, we propose a way to improve the sensitivity of the vector magnetic field sensing of the NV centers using multi-frequency control. Since the Zeeman energy of the NV centers depends on the direction of the axis, we can independently control the four types of NV centers using microwave pulses with different frequencies. This allows us to use every NV center for the vector field detection in parallel, which effectively increases the readout contrast. Our results pave the way to realize a practical diamond-based vector field sensor.The detection of small magnetic fields is important in the field of metrology, because there are many potential applications in biology and medical science. The performance of a magnetic field sensor is characterized by its spatial resolution and sensitivity; therefore, a significant amount of effort has been devoted to creating a device that can measure small magnetic fields in a local region [1][2][3].Nitrogen vacancy (NV) centers in diamond are fascinating candidates with which to construct a magnetic field sensor [4][5][6][7]. The NV center is a spin 1 system, and the frequency of the | ± 1 states can be shifted by magnetic fields. We can use this system as an effective two-level system spanned by |0 and |1 with a frequency selectivity where | − 1 is significantly detuned. We can implement gate operations of the spins in NV centers using microwave pulses [8][9][10][11]. It is possible to detect DC (AC) magnetic fields by implementing a Ramsey interference (spin echo) measurement [4][5][6]. Moreover, NV centers have a long coherence time, e.g., a few milli-seconds at a room temperature and a second at low temperature [12][13][14]. In addition, because the NV centers can be strongly coupled with optical photons, we can read out the state of the NV centers via fluorescence from the optical transitions [9,10]. The NV centers can be embedded in nanocrystals, which allows the NV centers to interact with local magnetic fields [15]. These properties are prerequisite to realizing a high-performance sensor for magnetic fields.Recently, vector magnetic field sensing by NV centers has become an active area of interest [16][17][18][19][20][21]. The NV center is aligned along one of four different axes due to C 3ν symmetry. The Zeeman energies of the NV centers are determined by gµ b B · d j (j = 1, 2, 3, 4) where g denotes the g factor, µ b denotes a Bohr magneton, B denotes the magnetic fields, and d j denotes the direction of the j-th NV axis. By sequentially performing Ramsey interference or spin echo measurements on NV centers with...