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In a small bowl, combine the smoked paprika, dried oregano, dried thyme, cayenne, garlic powder, onion powder, 1/2 tsp salt, and black pepper. Pat the shrimp dry with paper towels, then toss them with half of the spice blend and the coconut aminos until evenly coated. Set aside.
Heat a dry 12-inch skillet over medium-high heat until very hot. Add the tomatillos, jalapeño, and unpeeled garlic cloves (for the salsa verde) directly to the dry skillet. Cook, turning occasionally, until the tomatillos are charred in spots and softened, and the jalapeño skin is blistered, about 6–8 minutes. Transfer to a plate to cool slightly, then peel the garlic.
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