We demonstrate a bipartition technique using a superlattice architecture to access correlations between alternating planes of a mesoscopic array of spin-3 chromium atoms trapped in a 3D optical lattice. Using this method, we observe that out-of-equilibrium dynamics driven by long-range dipolar interactions lead to spin anticorrelations between the two spatially separated subsystems. Our bipartite measurements reveal a subtle interplay between the anisotropy of the 3D dipolar interactions and that of the lattice structure, without requiring single-site addressing. We compare our results to theoretical predictions based on a truncated cumulant expansion and a new cluster semiclassical method that we use to investigate correlations at the microscopic scale. Comparison with a high-temperature analytical model reveals quantum thermalization at a high negative spin temperature.