Pat the shrimp dry. Moisture is the enemy of good sear.
Lay shrimp on paper towels and blot well, then toss with 1 tablespoon oil.
Mix the seasoning. In a small bowl, combine chili powder, cumin, smoked paprika, oregano, 1 teaspoon salt, and 1/2 teaspoon black pepper. Sprinkle half over the shrimp and toss. Reserve the rest for the veggies.
Heat the pan. Place a large cast-iron or stainless skillet over medium-high heat.
Add 1 tablespoon oil.
Cook the peppers and onions. Add sliced peppers and onion with the remaining seasoning and a pinch of salt. Sauté 5–7 minutes, stirring occasionally, until slightly charred but still crisp-tender. Push to the edges of the pan.
Sear the shrimp. Add the remaining 1 tablespoon oil to the center.
Add shrimp in a single layer. Cook 1.5–2 minutes per side until opaque and just curled.
Add garlic and lime. Stir in the minced garlic for 30 seconds until fragrant. Squeeze in the juice of 1 lime and toss everything together.
Finish with cilantro. Remove from heat and sprinkle generously with chopped cilantro.
Taste and adjust salt, pepper, or lime.
Serve your way. Load into lettuce cups, spoon over cauliflower rice, or build a bowl with avocado, sour cream, cheese, and jalapeño. Add hot sauce if you like heat.