To directly investigate the correlation between magnetic moments along the honeycomb elements, we have performed polarized neutron experiments, namely reflectometry, off‐specular and grazing incidence neutron scattering (GISANS) measurements.21, 24, 25, 26 Together, they allow us to explore the underlying magnetic correlations27 at a length scale of ≈5 nm to 10 μm in the honeycomb lattice. In Figure 2 , we plot the off‐specular intensity measured using spin‐up (+) and spin‐down (−) neutrons at T = 300 K and 7 K. Here, the y‐axis represents the out‐of‐plane scattering vector Qz = 2πλ(sinαi+ sinαf) while, the difference between the z‐components of the incident and the outgoing wave vectors pi − pf = 2πλ (sinαi − sinαf) is drawn along the x‐axis. Thus, vertical and horizontal directions correspond to the out‐of‐plane and in‐plane correlations, respectively (for detail information, see Lauter et al.28). The specular reflectivity lies along the x = 0 line. Clearly, the off‐specular scattering plots show remarkable differences between high and low temperature measurements. At T = 300 K, the specular intensity is more than two orders of magnitude stronger compared to the off‐specular data, which is the expected behavior for most systems. There is also some scattering in the off‐specular regions caused by the paramagnetic nature of the moment and the honeycomb structure itself. The difference between the spin‐up and the spin‐down components in the off‐specular reflections is similar to that observed in the specular data (see Figure S1, Supporting Information). It indicates a paramagnetic or weak ferromagnetic character (MSLD = 5.9 × 10−6 Å−2 ↔ M = 1.92 × 105 A m−1) of the honeycomb lattice at room temperature. Upon cooling the sample to T = 7 K, the off‐specular signal increases significantly (notice the logarithmic color scale). No specular beam can be distinguished from the off‐specular background, anymore. As the nuclear structure factor will not change noticeably upon cooling, this can only be explained by a significant change in the magnetic characteristics of the system.