From what I've read, virtually all of the victims identified in the Family Secrets were trial were involved in the mob, save a few.

Explicitly, Arthur Morowski happened to be with Ortiz, and was murdered in cold blood. Frank Calabrese expressed regret over it but said he just "happened to be with the wrong guy a the wrong time."

Charloette Dauber was in some sense innocent, although reading between the lines it would be hard to believe that she did not know what her husband was involved in given his criminal record, and I believe she was also at least accused of engaging in some kind of criminal activity herself at one time. Still, the Calabreses expressed regret over it, with Nick blaming Frank and Frank, ridiculously, acting as if he wasn't part of it because he didn't himself pull the trigger.

There were a couple other victims who were not explicitly said to be involved in the mob, but, again, reading between the lines, I would imagine there is at least a good chance that they got their start with mobbed up money, etc., as the mob as far as I know generally does not go around randomly extorting legitimate businesses. But, I could be wrong.