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You have to complete the optional objects that contain a number of some sort, for example on the first mission the optional object you have to do is kill 100 grunts in a single game. After you complete the objective, watch your mini-map for a flare point (a pulsing circle), the center of that flare point is about where the skull is located. For compete details of objectives, and where the skulls are on each level see http://faqs.ign.com/articles/961/961650p1.html