Combine blood orange juice and simple syrup. Adjust sweetness according to taste.
In another container, combine lime juice, water and simple syrup. Adjust sweetness according to taste.
Divide blood orange among popsicle mold cavities. Place popsicle mold in the freeze. Tilt mold slightly to one side and prop it against something like an ice cube tray to keep it steady. Freeze for about 45 minutes until blood orange is solid.
Return popsicle mold to its upright position. Divide limeade among popsicle molds. Insert wooden sticks or paper straws into molds. Return mold to freezer and freeze for at least 4 hours until firm.