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Preheat oven to 350°F. Line 2 large rimmed baking sheets with aluminum foil or parchment paper.
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Combine chopped walnuts, flour, toasted coconut, baking powder, and salt in medium bowl and stir until well blended.
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Combine butter, chopped unsweetened chocolate, and 1 cup chocolate chips in heavy medium saucepan. Stir over low heat until butter and chocolate are melted and smooth. Remove saucepan from heat.
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Whisk instant coffee crystals and vanilla extract in medium bowl until coffee crystals dissolve. Add sugar and eggs. Using electric mixer, beat until mixture thickens, about 2 minutes. Beat in melted chocolate mixture, then chopped walnut mixture.
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Stir in remaining 1 cup chocolate chips and peanut butter chips.
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Mound 2 tablespoons dough for each cookie onto prepared baking sheets, spacing 2 inches apart.
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Bake cookies until puffed and cracked but still soft in center, about 15 minutes. Let cookies cool on sheets 10 minutes. Using spatula, transfer cookies to rack and cool.