First, make the coffee layer: In a large 6-8 ounce measuring cup, combine the cold brew coffee concentrate, mint-infused simple syrup, and Irish Cream (if using). Whisk gently to combine, and fill each of your popsicle molds about one-third to halfway up. Transfer any leftover coffee mixture to another container for another use (like drinking over ice, perhaps?) or discard.
Second, make the coconut cream layer: In the same measuring cup as the coffee layer (I don’t even bother to rinse it out since it’s all getting combined anyway), make the coconut cream layer by combining the can of coconut milk, half cup mint-infused simple syrup, and vanilla extract. Stir gently to combine the solids of the coconut milk with the rest of the mixture. The solids will float to the top of the mold, so if you want some more defined layers in your final pop, don’t whisk too much. If you’d rather a smoother popsicle, whisk until smooth.
Finish the popsicles: Gently pour this second cream layer into the molds on top of your coffee layer and fill to the top. Give each pop a gentle stir with a popsicle stick, and then place the popsicle mold into the freezer for one hour until partially frozen. Insert your popsicle sticks, and freeze an additional four hours until solid.
To un-mold: You can either store your popsicles in the mold until eaten, or remove them to store separately. To store separately, remove the mold from the freezer and let the popsicles sit for 5 minutes. Working quickly to avoid melting, remove each from the mold and wrap them in a strip of parchment paper. Place the wrapped pops in a freezer safe Ziploc bag or Tupperware container and store in the freezer. Enjoy your delicious popsicles within two weeks.