The time evolution of beam losses during a collimator scan provides information on halo diffusion and population. This is an essential input for machine performance characterization and for the design of collimation systems. Beam halo measurements in the CERN Large Hadron Collider were conducted through collimator scrapings in a dedicated beam study for the first time at 4 TeV. Four scans were performed with two collimators, in the vertical plane for beam 1 and horizontally for beam 2, before and after bringing the beams into collisions. Inward and outward steps were performed. A diffusion model was used to interpret the observed loss rate evolution in response to the collimator steps. With this technique, diffusion coefficients were estimated as a function of betatron oscillation amplitude from approximately 3 to 7 standard deviations of the transverse beam distribution. A comparison of halo diffusion and core emittance growth rates is also presented.