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A polycrystalline compact comprises a plurality of diamond grains of micron size, submicron size, or both, and a plurality of diamond nanoparticles disposed in interstitial spaces between the plurality of diamond grains. A method of forming a polycrystalline compact comprises combining a plurality of micron and/or submicron-sized diamond grains and a plurality of diamond nanoparticles to form a mixture and sintering the mixture in a presence of a carburized binder to form a polycrystalline hard material comprising a plurality of inter-bonded diamond grains and diamond nanoparticles. Cutting elements comprising a polycrystalline compact and earth-boring tools bearing such compacts are also disclosed.