I4 engines have extremely large second-order vibrations which give them the shakes. As far as V engines go, there is an ideal angle for the cylinders which results in maximum smoothness. For V6s, that angle is 60deg. 60deg V6s are very smooth. Many manufacturers make 90deg V6s, however, which are unbalanced, unless the crank journals are offset. 90deg is the 'magic' angle for a V8.
The smoothest engines are I6 - they have absolutely no first or second order harmonics to cause problems. And V12s, which are just two I6s together, are smooooth too.
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