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Preheat oven to 400º.
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Remove outer leaves from cauliflower and trim stem. Place on a large cutting board, stem side down. Starting at the center, cut into 1 inch thick slabs, retaining any florets that break off in the process.
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Coat a large skillet with 1 tablespoon of olive oil and place over medium-high heat. Working in batches if necessary, arrange cauliflower slabs and any stray florets in skillet and cook until lightly browned on bottoms, about 2 minutes. Flip and cook until browned on opposite sides, about 2 minutes more.
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Coat a large baking sheet with remaining oil. Arrange cauliflower on baking sheet and sprinkle with lime juice, garlic, cumin, ancho chili powder, salt and pepper. Bake until tender, about 15 minutes.