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In a blender, blend the watermelon, jalapeño, and sugar. Strain through a fine-mesh sieve into a pitcher. Add the tequila, Cointreau, and ½ cup lime juice + lime zest, stirring to combine. Pour the mixture among 6 popsicle molds or Dixie cups. Freeze one hour.
Rinse the blender out and blend the kiwi, cucumbers, 2 tablespoons lime juice, and 1 tablespoon tequila, blend until smooth. Pour the kiwi over the watermelon layer, filling the molds to the top. Insert popsicles sticks. Freeze until firm, at least 4 hours.
Serve with lime wedges and salt...and maybe even a margarita too!