Heat cream and chocolate together until melted and smooth. Cool at room temperature 1 1/2 to 2 hours, stirring occasionally, until spreadable.
Preheat oven to 350°F (175°C). Line two 8 or 9 inch round cake pans with parchment and grease.
Whisk flour, sugar, baking powder, baking soda, and salt in a large bowl.
Add eggs, oil, and buttermilk. Whisk gently until combined.
Mix boiling water with cocoa powder and instant coffee, then fold into the batter without overmixing.
Divide between pans and bake 20 to 28 minutes, until a toothpick comes out with moist crumbs.
Cool in pans 10 to 15 minutes, then turn out onto racks to cool completely.
Level the cake layers, fill and frost with the ganache.