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Preheat oven to 425°F. In a large bowl, combine the Brussels sprouts, orange zest, paprika, a pinch of salt and a few hefty grinds of pepper. Toss to combine. Drizzle with 1 to 2 tablespoons olive oil and toss again.
Line a baking sheet with non-stick aluminum foil. Drizzle lightly with olive oil and add salt and pepper to the pan. Add potatoes cut-side down. Spread Brussels sprouts mixture on top, then scatter with jalapeno slices. Roast until bright and golden, 30 to 35 minutes. Transfer to serving bowl and spritz with orange wedges to serve.