The effect of diamond surface treatment on the Thermal Boundary Conductance (TBC) between Al and diamond is investigated. The treatments consist in either of the following: exposition to a plasma of pure Ar, Ar:H and Ar:O, and HNO3:H2SO4 acid dip for various times. The surface of diamond after treatment is analyzed by X-ray Photoelectron Spectroscopy, revealing hydrogen termination for the as-received and Ar:H plasma treated samples, pure sp2 termination for Ar treated ones and oxygen (keton-like) termination for the other treatments. At ambient, all the specific treatments improve the TBC between Al and diamond from 23 ± 2 MW m–2 K–1 for the as-received to 65 ± 5, 125 ± 20, 150 ± 20, 180 ± 20 MW m–2 K–1 for the ones treated by Ar:H plasma, acid, pure Ar plasma, and Ar:O plasma with an evaporated Al layer on top, respectively. The effect of these treatments on temperature dependence are also observed and compared with the most common models available in the literature as well as experimental values in the same system. The results obtained show that the values measured for an Ar:O plasma treated diamond with Al sputtered on top stay consistently higher than the values existing in the literature over a temperature range from 78 to 290 K, probably due a lower sample surface roughness. Around ambient, the TBC values measured lay close to or even somewhat above the radiation limit, suggesting that inelastic or electronic processes may influence the transfer of heat at this metal/dielectric interface.