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The exceptionally high thermal conductivity of polycrystalline diamond (∼2000Wm-1K-1) makes it a very attractive material for optimizing the thermal management of high-power devices. In this paper, the thermal conductivity of a diamond sample capturing grain size evolution from nucleation towards the growth surface is studied using an optimized 3ω technique. The thermal conductivity is found to decrease with decreasing grain size, which is in good agreement with theory. These results clearly reveal the minimum film thickness and polishing thickness from nucleation needed to achieve single-crystal diamond performance, and thus enable production of an optimal polycrystalline diamond for heat-spreading applications.