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Preheat the oven to 180°C (160°C fan/Gas Mark 4). Grease and line two 20 cm round cake tins with baking parchment.
In a large bowl, cream together 200 g unsalted butter (softened) and 200 g caster sugar until light, pale and fluffy.
Crack in 4 large eggs, one at a time, beating well after each addition (add a spoonful of flour if the mixture looks curdled).
Stir in the coffee mixture: 2 tablespoons instant coffee granules dissolved in 2 tablespoons hot water and cooled.
Gently fold in 200 g self-raising flour until just combined.
Stir in 100 g walnuts (roughly chopped) until evenly distributed.
Divide the batter evenly between the two prepared tins and smooth the tops. Bake for 20–25 minutes, or until golden brown, springy to the touch, and a skewer inserted into the centre comes out clean.
Allow the cakes to cool in their tins for 10 minutes, then turn out onto a wire rack to cool completely.
To make the buttercream, beat 150 g unsalted butter (softened) until creamy. Gradually add 300 g sifted icing sugar, beating well after each addition. Stir in the coffee mixture (1 tablespoon instant coffee granules dissolved in 1 tablespoon hot water and cooled) and 1.5 tablespoons milk. Beat on high speed until light, fluffy and spreadable.
Place one cooled sponge on a serving plate. Spread half the buttercream over the top, then top with the second sponge. Spread the remaining buttercream over the top and decorate with walnut halves.