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Easy one this, Matra V12, sounded awesome, infact it sounded so good that it wasnt that great as an F1 engine, all the horses were wasted on creating the soundtrack!!
Going on to more modern engines I always liked the scream of the V10s, the current V8s sound muted by comparison, infact the move from V10s to V8s strikes me as the most pointless move in recent F1 history as all it did was ensure the most costly way possible to achieving parity in engine power.
Also the Honda and Ferrari 3.5 litre V12s sounded fantastic, the Honda had a lovely throaty bottom end twinned with a high rev scream.