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In a small bowl, combine the chili powder, cumin, smoked paprika, garlic powder, onion powder, oregano, salt, and pepper. Pat the chuck roast dry with paper towels, then rub the spice mixture evenly over all sides.
Heat the olive oil in a large skillet over medium-high heat until shimmering. Add the roast and sear, undisturbed, for 3–4 minutes per side until a deep brown crust forms on each surface, then transfer to the slow cooker insert.
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