These two questions are actually asking about two different actions. The first asked how to undo adding a user to a group. The second asked how to remove a user entirely from the system.
For the former, you can just invoke the same usermod command with -r instead of -a.
For the latter, install shadow-userdel and invoke userdel as usual.
Another option: With any text editor (vi if everything else fails) directly manipulate or delete the respective lines from
/etc/passwd for users and their cornerstone data
/etc/shadow for their passwords (i.e., housekeeping)
/etc/groups for user groups
AFAIK the dedicated tools to add and remove users are mainly for convenience and to manipulate the system at runtime (e.g., bumping logged in users off the system when they are removed).