Polycrystalline compacts include an interface between first and second volumes of a body of inter-bonded grains of hard material. The first volume is at least substantially free of interstitial material, and the second volume includes interstitial material in interstitial spaces between surfaces of the inter-bonded grains of hard material. The interface between the first and second volumes is configured, located and oriented such that cracks originating in the compact during use of the compacts and propagating along the interface generally toward a central axis of the compacts will propagate generally toward a back surface and away from a front cutting face of the compacts at an acute angle or angles. Methods of forming polycrystalline compacts involve the formation of such an interface within the compacts.