They're both 4 cylinder motors without modern tech like balance shafts, electronically controlled engine mounts, etc.
4 cylinders from the W124 era are inherently lacking smoothness.
If it is smoothness you're after, you need to step up to at least a 6 cylinder. Also, the M102 has to work hard to move the mass of the W124 and revs high on the highway.
FWIW, think of the M111 as a upgraded M102. The M111 bases its roots on the M102 in a similar way as does the M104 to the M103.